1-s2.0-S2590123022003413-main

Results in Engineering 16 (2022) 100671
Contents lists available at ScienceDirect
Results in Engineering
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A review of emerging micro-pollutants in hospital wastewater:

Environmental fate and remediation options
O.J. Ajala a, c, *, J.O. Tijani a, c, R.B. Salau a, c, A.S. Abdulkareem b, c, O.S. Aremu d
a
Department of Chemistry, Federal University of Technology, P. M. B. 65, Bosso Campus, Minna, Niger State, Nigeria
b
Department of Chemical Engineering, Federal University of Technology, P. M. B. 65, Gidan Kwano Campus, Minna, Niger State, Nigeria
c
Nanotechnology Research Group, Africa Center of Excellence for Mycotoxin and Food Safety, Federal University of Technology, Minna, P. M. B. 65, Niger State, Nigeria
d
Department of Chemistry and Biochemistry, University of Windsor – Ontario Canada 401 Sunset Avenue Windsor, Canada
A R T I C L E I N F O A B S T R A C T
Keywords: Hospitals played vital role in the maintenance and sustenance of human health. However, hospital activities
Hospital wastewater hazards generate high volume of toxic solid and liquid containing diverse inorganic, organic and microbial wastes
Ciprofloxacin released untreated into the ecosystem. The management of hospital wastewater in particular has been a major
Orfloxacin
source of concern due to the presence of unregulated emerging micro-pollutants at concentrations in the range of
Norfloxacin
Carbamazine
ng/L to μg/L. These pollutants at low concentration exert different potential health effects on human and aquatic
Clofibric acid species. In this review, the formation, composition, properties and ecotoxicology effects of selected emerging
Adsorption micro-pollutants (Norfloxacin, Ofloxacin, Ciprofloxacin, Clofibric acid and Carbamazepine) at different con
Advanced oxidation processes centrations in hospital wastewater were reviewed. The review also elucidates on detection and quantification of
concentration of different emerging micropollutants in hospital wastewater by Spectrophotometry techniques,
Gas Chromatography, Ion Chromatography, Gas Chromatography-Mass spectrometry, and High-Performance
Liquid Chromatography. Furthermore, treatment of hospital wastewater through physical, biological, chemi
cal, adsorption and advanced oxidation processes such as photocatalysis and photo-Fenton including their
operational mechanism were provided. The chemistry and mechanism of degradation of the selected emerging
micropollutants into several intermediates were reviewed. It was found that conventional wastewater treatment
methods are not designed for effective removal of these unregulated pollutants in hospital wastewater because
they exist as mixtures at very high concentrations and exerts different toxicological effects. The review also
reveals that no single technology can effectively detoxify the wastewater, instead combination of methods such
as (phototcatalytic/adsorption or photo-fenton/adsorption) was found most appropriate for hospital wastewater
treatment. Finally, regular monitoring and determination of physicochemical and ecotoxicological parameters
and treatment of hospital wastewater are recommended.
namely laundry, kitchen, number and type of wards and units, tem
1. Introduction perature control systems; numbers of outpatient and inpatients; facility
age, number of beds, and maintenance procedures; institutional man
Hospitals played critical role in the maintenance of the health status agement practices, geographic location, period of services, and season
of a country citizen. On the other hand, hospital activities are often all have impacts on the volume of wastewater generated in any hospital
accompanied with the generation of diverse inorganic, organic and [3]. The water consumption in hospitals has been estimated between
microbial components usually released without prior treatment into the 200 and 1200 L per bed per day, with highest values obtained from
environment. Hospital waste management has been a major source of developed nations and the lowest from developing countries (200–400
concern to the environmental chemist due to the presence of toxic L/bed/day) [4]. In industrialized countries, total hospital wastewater
contaminants that exerts harmful impacts on human and aquatic spe output range from 250 to 570 m3 per day, with a fraction of hospital
cies. According to Ogwugwa et al. [1], daily wastewater generated in the wastewater ranging from 0.2 to 65% flown and processed in municipal
hospital per bed varies from 40 to 120 L in developed countries and wastewater treatment facilities [4].
2–50 L in developing countries like Nigeria [2]. Existing general services Hospital wastewater is loaded with several emerging micro-
* Corresponding author. Department of Chemistry, Federal University of Technology, P. M. B. 65, Bosso Campus, Minna, Niger state, Nigeria.
E-mail address: [email protected] (O.J. Ajala).
https://doi.org/10.1016/j.rineng.2022.100671
Received 21 July 2022; Received in revised form 23 September 2022; Accepted 23 September 2022
Available online 28 September 2022
2590-1230/© 2022 Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
O.J. Ajala et al. Results in Engineering 16 (2022) 100671
using characteristics such active component intake, water consumption

Abbreviation per bed, and percentage excretion [9]. Exposure to these pharmaceuti
cally active residual compounds has contributed to the increasing anti
AOP Advanced oxidation processes biotic resistance, as most bacteria and fungi have ability to destroy the
BPC Base Peak Chromatogram drugs. For instance in United States of America (USA) alone, approxi
CA Clofibric Acid mately 2.8 million antibiotic-resistant infections and 35,000 deaths have
CIP Ciprofloxacin been reported yearly, thus considered as emerging areas of concern.
CBZ Carbamazepine, Most municipal wastewater treatment plants are designed for the
DNA Deoxyribonucleic Acid removal of biodegradable compounds such as, carbon, phosphorus, and
EC50 Half Maximal Effective Concentration nitrogen molecules, as well as microorganisms, but not micro-pollutants
EIC Extracted Ion Chromatogram such as chemical and pharmaceutical residues, and endocrine disrupting
GC-MS Gas Chromatography Mass Spectrometry compounds [9]. However, Chlorination is sometimes required for the
HPLC High Performance Liquid Chromatography treatment of the total hospital wastewater, and other times the treat
NGOs Non Governmental Organization ment is just required for the effluent from infectious disease units before
NOR Norfloxacin being discharged into the municipal sewer [13].
NOEC No Observed Effect Concentration Many authors believe that treating urban and hospital wastewaters
OFL Ofloxacin in a municipal effluent treatment plant is ineffective because it relies on
PEC Projected Environmental Concentration dilution of diverse outputs and did not allow for pollutant isolation [14,
pH Potential Hydrogen 15], particularly emerging micro-pollutants and dangerous compounds,
TIC Total Ion Count from the liquid phase [16]. Micro-pollutants, particularly pharmaceu
TCS Triclosan ticals, are difficult to remove from wastewaters because their concen
UTI Urinary Tracts Infections trations are in the range of 10− 3–10− 6 mg/L, which is significantly lower
UV–Vis Ultraviolet Visible Radiation than that of traditional macro pollutants (COD, BOD5, phosphorus and
nitrogen compounds) [17]. Furthermore, emerging micro-pollutants
encompass a wide range of compounds with significant variances in
their primary features, which influence their behavior and fate in the
pollutants such as; original or metabolized pharmaceuticals compounds wastewater treatment process. The biodegradability and physicochem
such as anti-inflammatory, anti-diabetic, antiepileptic, pesticides res ical qualities such as; water solubility, adsorption, and volatilization of
idue, industrial chemicals, perfluorinated compounds, surfactants, per typical pollutants found in hospital wastewater determine their removal
sonal care products, analgesics, disrupting compounds, endocrine, effectiveness [18]. The features of wastewater treatment plants (that is,
antibiotics and hormones radioactive elements, and microorganisms tertiary, secondary and primary treatments), operating circumstances
such as; fecal coliform, total coliform, pathogens (E. coli, Vibrion (sludge retention time, temperature, pH and hydraulic), reactor type,
Staphylococcus aureus, Salmonella, and Pseudomonas aeruginosa), radio- and other variables are affected by biodegradability and physicochem
elements, and heavy metals [5]. Some of these pollutants are catego ical qualities [6]. Since there are new analytical standards which are
rized as micro-pollutants (10− 6 –10− 3 mgL− 1) or macro-pollutants commercially available; the number of emerging micro-pollutants based
(>10− 3 mgL− 1) based on their measured quantities, and the majority on recent investigations continue to increase, and more than 300
have no regulatory status in the environment [6]. pharmaceutical residues and conjugates chemical have been identified.
Of particular interest are the emerging micro-pollutants, these are Current researches have been to conduct health risk assessment of
natural or synthetic substances not routinely monitored in the envi number of compounds, because of growing evidence of possible influ
ronment but have the potential to infiltrate and exert different health ence on aquatic creatures (such as organ abnormalities, genetic lesions,
problems [7]. These chemicals enters the ecosystem through different reproductive abnormalities, and behavioral alterations) and
point and non-point sources such as release of untreated wastewater antibiotic-resistant genes and bacteria [19], thus, these pollutants are of
generated, half used and expired products, manufacturing processes and special concern.
excretion of partially mineralized drugs from the body into sewer system Owing to various problems of hospital wastewater and its derivative,
[8]. Drugs with active ingredients are metabolized after administration several conventional methods such as; chlorination [20], ozonation
and the unmetabolized active substances are excreted either unaltered [21], reverse osmosis [22], activated carbon adsorption [23],
compounds, or conjugated with an deactivating agent or a combination ultra-filtration [24], electro-coagulation [8] have been applied for their
of metabolites linked to the molecule [9], For instance, urine accounts removal from wastewater. However, each of the methods has different
for 55–80% of the total unmetabolized active ingredients [10] and associated setbacks. For instance, chlorination technology often lead to
partially in faeces, and thus enter the water cycle. Waste generated from formation of disinfection by-products (DBPs) which are very more
laboratory, diagnostic unit, and operating theater through patients make harmful and carcinogenic to human being [25]. Ozonation, and reverse
hospitals key providers of these wide range of micro-pollutants [3]. osmosis are very costly [26]. Adsorption technology always generates
Chemicals, disinfectants, heavy metals, and sterilizants, iodinated toxic sludge which occupies space during processing [27]. All these
contrast media, and radioactive markers are among the active principles setbacks make it difficult to achieve the desired treatment of
of medications and their metabolites [3]. wastewater.
Hospital effluents have a toxicity that is 5–15 times that of an urban On the contrary, advanced oxidation processes (AOPs) have been
effluent and this constitute serious human and environmental risks found suitable for successful removal and degradation of toxicants/
following organisms exposure to hazardous substances, or infiltration pollutants through generation of oxidizing agent (hydroxyl radicals or
into groundwater [11,12]. Hospitals, on the other hand, are not the only other free reactive species) [28]. Different researchers have studied
source of pharmaceutical residues found in all wastewater treatment degradation of hospital wastewater and its derivatives (such as tetra
plants due to their micro properties [6]. Regardless of their variations, in cycline antibiotic, Phenol Forrnaldehyde, Choramphenicol, Norfloxacin,
most cases, hospital effluents are categorized as having the same Ciprofloxacin, Dichlofenac, Acetaminophen and Atenolol) using photo
pollution load as sewer wastewaters and are released into public sewage catalytic technology [29], Electro-oxidation [30], Electro-fenton [30],
systems, and received as an urban wastewater in treatment facility, and Electrocatalysis [31], Ozonation [26], Photo-Fenton [32], Metallic
treated in the same manner. The predicted concentrations or observed Nanoparticles [33], and Fenton reaction [34]. Most of these techniques
values of pharmaceutical residues in hospital wastewater are calculated are capable of degrading various pollutants nevertheless their efficiency
2
is low [35,36]. such as platinum via excretion by Oncology patients who have been
Recently, research attention has shifted to hybrid/combination of given cis-platinum, carboplatinum, or other cytostatic drugs. [40];
different treatment techniques to achieve the desired degradation effi Mercury is widely found in disinfectants, diagnostic agents, and di
ciency of emerging micro-pollutants in hospital wastewater within short uretics as active components [5]; and due to gadolinium large magnetic
period of time. In this review paper, the following emerging micro moment, it is often found in iodinated contrast medium used in magnetic
pollutants namely Norfloxacin, Ofloxacin, Ciprofloxacin, Clofibric acid, resonance imaging [41]. Mercury, and platinum are the most common
Carbamazepine were selected due to their increase prevalence in the heavy metals detected in hospital effluents [39]. Other heavy metals,
water bodies across the world coupled with the growing cases of bac such as copper, lead, cadmium, iron, and nickel, are commonly found in
terial infections rate among patients. Norfloxacin, Ofloxacin and Cip municipal wastewater at similar amounts [39,42–44]. Due to the high
rofloxacin all belong to quinolone antibiotics family used for the magnetic moment imaging of the digestive system, with three magnetic
treatment of bacterial related infections especially such as urinary tract resonance imaging systems serve 15 to 25 patients on a daily basis, spine
infections (UTI). Specifically, Norfloxacin is applied primarily to subdue (MRI), and brain, gadolinium-containing compounds such as gado
spontaneous bacterial peritonitis (SBP) in patients with liver cirrhosis pentetic acid, gadodiamide, and Gd-diethylenetriamine pentaacetate are
while Ciprofloxacin is also known for curing SBP in patients. Studies delivered (intravenously or orally) regularly. After a few hours of
have shown that UTI is one of the most globally prevalence health administration, the contrast media are excreted unmetabolized into
problem especially among women and out of 8 million patients in one hospital sewage. It was established that approximately 90% of gado
each year, 10 in 25 women and 3 in 25 men usually have symptoms of a linium is eliminated during the patient’s stay in hospital within 24 h
UTI. Clofibric acid is an antilipemic agent used for the treatment of [45], while at home, an excretion rate of 85–98% within 70 min may be
hypertrigly ceridemia and high cholesterol. Carbamazepine is a drug achieved. For instance, Oliveira et al. [46], detected gadolinium in
used for the treatment of patients’ diagnosed with epilepsy and severe effluent from Freiburg University Hospital Germany. Mercury is
diabetes (peripheral neuropathy). It is estimated that 5 million in commonly found in agents of diagnostic, disinfecting active compo
dividuals worldwide are diagnosed with epilepsy each year. Epilepsy is nents, and agents of diuretic. In hospital wastewater, mercury contents
estimated to affect 49 persons out of every 100,000 in high-income vary from 0.3 to 7.5 g/L [47]. Since the early 2000s, developed nations
nations each year. Each year, 139 people in middle and low-income have made an attempt to decrease mercury pollution by adopting
nations are diagnosed with epilepsy. diagnostic agents without this heavy metal and establishing improved
Thus, to the best of our knowledge, this is the first review on waste management techniques.
occurrence, environmental fate, quantification of the selected emerging Since the mid-1970s, platinum-containing compounds such as; car
micro-pollutants in hospital wastewater. The review also provides boplatin and cisplatin, have been utilized as anti-neoplastics in oncology
insight on the different analytical methods for the detection and quan [46]. These antineoplastics are eliminated at various rates after
tification of the emerging micro-pollutants. The review also provides an administration (patient dependent). Within the first 24 h following
overview of the conventional methods of treating hospital wastewater administration, Carboplatin is excreted in 50–75% rate [46]. Cisplatin is
namely: the physical, biological and chemical counterpart. In addition, excreted between 31 and 85% rate within 51 days after treatment. The
the review also focus on the theory, mechanism and application of two long-term stages of platinum renal excretion have biological
advanced oxidation processes such as photocatalysis, photo-Fenton and half-lives of 160 and 720 days, respectively. 70% of the platinum given
combined advanced treatment techniques for the removal of the selected is anticipated to be excreted in hospital wastewater [46]. The platinum
micro-pollutants in hospital wastewater. This state-of-art review also content was measured by Kümmerer et al. [48], in five European hos
outline new insights on the mechanisms and degradation of the selected pitals of various sizes and found to vary between 174 and 2514 beds
emerging micropollutants and formation of various intermediates based with concentrations ranging between 3.5 and 0.01 g/L. The authors
on the adopted treatment method. examined the fluctuation in platinum concentration in the Freiburg
University Hospital, Germany over the period of 24 – hour and discov
2. Formation and composition of hospital wastewater ered two concentration maxima at 10 a.m. and 4 a.m. Platinum temporal
variability was measured for one week at the main building of the
Hospital wastewater encompasses varieties of conventional and non- Geneva University Hospital (741 beds – Switzerland) by Daouk et al.
conventional parameters based on the geographical locations. The for [49], who found a significant rise at the end of the week. Platinum
mation and compositions (Bacteriological, heavy metals and Pharma concentrations were measured between 0.01 and 2 gL-1 and a ranged of
ceutical residues) are discussed in this section. 2.0–289 g/L was found in an oncological unit in Vienna, Austria [50].
They carried out a platinum speciation study and discovered that car
2.1. Bacteriological composition boplatin was the major cause of Platinum loading.
The evaluation of markers of fecal contamination and pathogens is 2.3. Pharmaceutical residues composition
usually included in the bacteriological composition of hospital waste
water. E. coli is generally used to identify fecal coliforms since it ac The use of medicines varies greatly amongst healthcare institutions
counts for 80–90% of thermo-tolerant coliforms identified [37]. E coli is [51]. For instance, the entire pharmaceutical consumption of a nursing
a kind of facultative anaerobic bacterium found in the stomach and home, a mental hospital, and a regular hospital in Germany has been
feaces. The presence of E coli in hospital wastewater indicates fecal calculated and varied from 32 kg/year (hospital of psychiatric) to 1263
pollution, and besides E coli, other harmful fecal microorganisms such as kg per year (general hospital), with yearly average pharmaceutical
spores of sulfite-reducing anaerobes, Staphylococcus aureus, Salmonella consumption ranges between 0.1 and 1000 g per bed [5]. Contrast
typhii, Pseudomonas aeruginosa; and pathogenic viruses (rotavirus, nor media, analgesics, antibiotics, laxatives, anti-inflammatories, and cyto
ovirus, enterovirus, adenovirus) and hepatitis A virus are also exist in static medicines are the most commonly used therapeutic categories in
high proportion in hospital wastewater [1]. Thus, Enterovirus concen hospitals [52].
trations have been shown to be 2–3 times higher in hospital wastewater Pharmaceutical residues in hospital wastewater are determined by a
than in municipal wastewater [38]. combination of three primary factors: the amount given, the fraction
excreted, and the chemical properties (primarily biodegradability and
2.2. Heavy metal composition stability) [53]. In diverse geographic locations, hospital wastewater
have been tested for pharmaceutical residues (Asia – [54], Europe –
Different heavy metals have been found in hospital wastewater [39], [55], and North America – [56].
3
Mayoudom et al. [56], reported the analysis of 12 pharmaceuticals in cephalosporins. Penicillins and carbapens are two more groups with
hospital wastewater and found to have the concentration in range of 78 substantial anticipated concentrations with 262 μg/L and 229 μg/L
μgL− 1 and 5 mgL− 1. The percentage distribution of therapeutic cate respectively. Ampicillin (222 μg/L) and meropenem (220 μg/L) had the
gories is dependent on the analyte under investigation, which usually highest anticipated concentrations within these two groups [67]. Ac
account for 94% of the total concentrations tested. The most common cording to de Souza et al. [64], the majority of the intravenous antibi
treatment groups are contrast media, analgesics, cytostatics, and otics studied pose a significant environmental risk. Some of the hazards
anti-infective and anti-bacterials, which account for more than 40% of associated with antibiotic release are due to the emergence of
the total concentration observed in hospital wastewater [3]. Other antibiotic-resistant microorganisms [68].
identified classes of pharmaceuticals detected include anti-epileptic, These antibiotics contain adsorbable organic halides, volatile
psychoanaleptic, anti-inflammatory, and -blocker medications with a organic and other organic compounds such as phenol, alcohols, acetates,
maximum concentration of 20% of the total concentration tested [3]. ketones and acetaldehyde [69]. Adsorbable organic halides can be found
The majority of pharmaceuticals found in hospital wastewater had in pharmaceuticals and disinfectants formed from chlorine applied in
maximum values of less than 10 g/L [57]. Higher concentrations are cleaning, halogen-containing solvents, and other forms chemical like
usually detected for particular chemicals (such as; ibuprofen, acet ethidium bromide [37]. In hospital wastewater, adsorbable organic
aminophen, ciprofloxacin, caffeine, iomeprol, gabapentin, iopamidol, halides levels range between 150 and 7760 μgL− 1, in contrast to the 0.04
iopromide, theobromine, metformin), with numerous contrast media to 0.2 μgL− 1 range reported in urban wastewaters [37].
agents at the low concentration in mgL− 1 range [9]. Daouk et al. [49],
examined different categories of pharmaceuticals in Geneva University 2.4. Concentrations of pharmaceutical residues in the hospital wastewater
Hospital Switzerland with beds of 741 capacities and calculated mean
daily loads to be between 0.1 and 14 g/day for 15 pharmaceuticals, Predicted and measured concentrations of pharmaceutical residues
except for piperacillin (0.08 g per day), acetaminophen (143 g per day) in hospital wastewater may provide different findings with respect to the
and diclofenac (0.04 g per day). The weekly variability of these medi time frames used. Projected concentrations are extrapolated from yearly
cines was explored, and daily load for compounds like morphine, pharmaceutical usage statistics in most circumstances, whereas con
ibuprofen, and acetaminophen, which are often taken on a regular basis, centrations are established for a certain time period and at a single point
stayed between 50 and 150% of the average [58]. Pharmaceuticals less in time [5,70]. Depending on the chemicals, measured concentrations
often used, are mefenamic acid, diclofenac, and the anti-epileptics may have more variability than anticipated values. Predicted concen
gabapentin, however have a larger variability, up to 400% of the trations are considered by some authors to be a superior choice for
average value, with the greatest concentrations recorded during the determining pharmaceutical discharge over extended time periods [40].
week. Among the medicines studied metronidazole showed more vari Each technique has advantages and disadvantages that should be
ability than sulfamethoxazole and ciprofloxacin with the greatest considered when building a source characterization attempt. The choice
amounts of metronidazole detected early in the week. between the two is ultimately determined on access to consumption
Compared to general hospitals, specialized wards and hospitals such statistics, cost, and sewage system accessibility, as well as research
as; oncologic unit, critical unit, geriatric unit, and psychiatric unit goals.
employ a diverse set of medicines. Anti-metabolites and anthracyclines Prioritization approaches have been created because the medications
were found in the wastewater of an oncological in-patient care unit (18 are commercially available in hundreds, and many of them can be
beds) at Vienna University Hospital, Austria [50]. In the treatment of discovered in the ecosystem as conjugates or parent molecules. These
lung, bladder, breast, and cutaneous cancer, the anti-metabolite 5-fluo prioritization approaches take into cognizance varieties of parameters
rouracil is given in doses ranges between 200 and 1000 mg/m2 body such as physico-chemical properties, degradability/persistence, con
surface [59]. Within 24 h, around 2–35% of the given medication was sumption/sales, (eco) toxicity risk, and treatment resistance [6]. Table 1
found unmetabolized in the patient urine [59]. Epirubicin, doxorubicin, summarizes various concentration of micro-pollutants (therapeutic
daunorubicin, and anthracyclines, are commonly used to treat solid and drugs) observed in the healthcare facilities effluents. According to this
hematological tumors, such as high-grade lymphoma, acute leukemia, table; there are different classification of pharmaceutical residues such
bladder cancer and breast cancer, at doses ranges between 15 and 120 as; Analgesics/inflammatory, antibiotics, anti-hypertensive, psychiatric,
mg/m2 body surface [60]. Within 24 h, approximately 3.5–5.7% of beta-blocker, hormones and contrast media. In analgesics, paracetamol
doxorubicin, 13–15% of daunorubicin and 11% of epirubicin were was reported to range between 5 and 1,368, ibuprofen between 0.07 and
found unmetabolized in the urine [61]. 5-Fluorouracil and doxorubicin, 43, codeine between 0.02 and 50. In antibiotics, ciprofloxacin was re
which were given as cytostatics, were detected in the wastewater be ported to range from 0.03 to 125 and norfloxacin between 0.33 and
tween 8.6 and 124 μg per Lit and 0.26 and 1.35 μg per Lit respectively 44.00.
[62]. The wastewater of the oncological in-patient treatment ward [3].
contained 0.5 to 4.5% of the administered quantity of 5-fluorouracil and
0.1 to 0.2% of the administered amount of doxorubicin [63]. 3. Adverse effects of hospital wastewater on environment
de Souza et al. [64], examined intravenous antibiotics used in a
Brazilian hospital’s intensive care unit (16 beds) and equally estimated Pharmaceuticals are excreted as a combination of unmodified parent
the environmental risk and projected environmental concentration chemicals and their intermediates (that is metabolite) following inges
(PEC). The usage of antibiotics in the critical care ward is significant tion. Although it may appear intuitive that a highly degradable sub
because, this unit consumed 25% of all antibiotics even though the unit stance (one with a low excretion rate) is easier to break down in the
occupies only 10% of the hospital’s entire number of beds are available. ecosystem, studies have found a negative correlation between the pro
Several intravenous antibiotic classes were utilized, with piperacillin, portion of excreted pharmaceuticals and their concentration in the
ceftriaxone, ampicillin, meropenem, ceftazidime, cefazolin, sulbactam, ecosystem, implying that poorly excreted pharmaceuticals may have a
clindamycin, trimethoprim, cefepime, and vancomycin having the low environmental degradability inherently [71]. Pharmaceuticals may,
greatest usage [65]. These researchers computed PECs by taking into in fact, take a variety of paths once they enter the sewage system,
account effluent dilution due to surface water flow (10 times) [5]. The exhibiting great environmental stability and permanence, or volatiliza
estimated concentrations discharged by the critical care unit vary be tion, and chemical or biological degradation. Drugs such as ciprofloxa
tween 1.15 μgL− 1 for quinolones to 701 μgL− 1 for cephalosporins, if the cin and ceftazidime which contain both basic and acidic functional
dilution effect is ignored [66]. Ceftriaxone (320 μg/L) and cefazolin groups exhibited more complex behavior in sewer network, as well as
(280 μg/L) have the highest anticipated concentrations among during wastewater treatment. This means that, depending on the
4
Table 1 To make matters even more complicated, concentrations of some

Micro-Pollutants: Concentration of Classes of Therapeutic Drugs Measured in pharmaceuticals have been discovered between the technique’s limit of
Healthcare Facilities wastewater. quantification and detection, and consistently below the projected
Classification/Analyzed compounds Concentrations (μg/L) concentration of the environment. This happened, for example, with the
Analgesics/Anti-inflammatories
anti-neoplastic drug tamoxifen [75], and could be attributed to one or
Paracetamol 5.00–1368 many reasons in this case. One theory is that tamoxifen gets deteriorated
Ibuprofen 0.07–43.00 before being analyzed because the compound is reported to be UV ra
Codeine 0.02–50.00 diation sensitive, degrading by up to 90% in just 5 days [75]. Photo
Naproxen 10.00–11.00
degradation could not be completely prevented in this case, despite the
Diclofenac 0.24–15.00
Salicylic acid 23.00–70.00 fact that the analysis was performed as rapidly as feasible and the
samples were shielded from light in the meanwhile. Tamoxifen’s high
Antibiotics
lipophilicity (measured log Kow = 6.3) allows it to easily bind to particle
Ciprofloxacin 0.03–125 detritus that settles to the bottom of sewage systems, avoiding detection
Metronidazole 0.10–90.00
[76].
Tetracycline 0.01–4.00
Ofloxacin 0.35–35.00 Another explanation for the discrepancy between measured and
Clarithromycin 0.20–3.00 expected tamoxifen concentrations could be an overestimation of PEC
Norfloxacin 0.33–44.00 due to the adoption of an improperly inflated unaltered compound
Penicillin 0.85–5.00 excretion rate [77]. After the treated wastewater passed through treat
Doxycycline 0.10–7.00
Oxytetracycline 0.01–4.00
ment plants, the remaining active pharmaceutical ingredients may
Erythromycin 27.00–83.00 degrade further in surface water bodies. Indeed, if a substance is sensi
Sulfamethoxazole 0.04–83.00 tive to light, photodecomposition may aid the degradation in the envi
Lincomycin 0.3–2.00 ronment. Phototransformation is straightforward in clear surface water,
Trimethoprim 0.01–15.00
and the efficiency of the process is proportional to the frequency and
Anti-hypertensive intensity of available light [78]. Other variables, such as water hardness,
Diltiazem 0.71–2.00 pH, season, location, and latitude, may, however, influence this process
[79]. Despite the fact that tetracyclines, quinolones, and sulphonamides
Psychiatric
among others are light-sensitive antibiotics, not all antibiotics are
Carbamezepine 0.54–2.00
photodegradable [80]. Indeed, relevance of each antibiotics and their
Beta – blockers amount of direct and indirect photolysis in the aquatic ecosystem are
Metoprolol 0.45–25.00 different. Therefore, there is need to review the following selected
organic pollutant; norfloxacin, ofloxacin, ciprofloxacin, clofibric acid
Hormones
and carbamazepine due to their high rate of consumption which result to
Estrone, E1 0.02–0.03
their recalcitrant and persistence nature in environment most especially
Ethinylestradiol, EE2 0.02–0.02
17β – estradiol, E2 0.03–0.04
in hospital wastewater.
Estriol, E3 0.35–0.50
Contrast media
3.1. Norfloxacin (NOR)
Iomeprol 0.01–1392
This is one of the most widely used anti-infective drugs globally with
Iopromide 0.2–2500
a brand name of noroxin, among others. It belongs to the class of fluo
Anti-cancer
roquinolone antibiotics which is used to treat gynecological infection,
5 – fluorouracil 5.00–124 urinary tract infection, gonorrhea, inflammation of the prostate gland
Cyclophosphamide 0.008–2.00 and bladder infection [81]. Humans and cattle only partially metabolize
Ifosfamide 0.01–2.00
the drug, with a significant portion expelled in urine and feaces and
Tamoxifen 0.004–0.17
released into urban wastewaters, sewage sludges and manures, posing
Anti-diabetics
additional environmental hazards [82]. Norfloxacin has the potential to
Glibenclamide 0.05–0.11 harm aquatic ecosystems by limiting algae reproduction and survival
Anti-viral [83], reducing Daphnia sp swimming capacity and predation rate [81],
as well as creating functional and structural alterations in plankton
Aciclovir 0.02–0.60
systems, according to some laboratory experiments [84]. Norfloxacin
can affect aquatic organisms through alteration of antioxidant enzymes,
ambient conditions, behavior of these molecules can behave as anionic, causing considerable DNA damage, and exert genotoxic and cytotoxic
cationic, neutral, or zwitterionic in the environment [71]. As a result, effects [85]. Antibiotics’ effects on the soil system, on the other hand,
understanding the physicochemical features of pharmaceutics can aid in are little known. Antibiotic concentrations of up to 10 mg/kg have been
predicting the activities that occur during their passage through found in manures, with concentrations approaching the mg/kg level in
wastewater treatment plants. These processes may include biodegra manure-amended soils [86]. After manure amendment, most
dation, or chemical transformation, sorption onto solids, and residual soil-dwelling organisms are expected to encounter 5–10 mg/kg of
pharmaceuticals may be exposed to photolysis and photodegradation antibacterial compounds in soils [86]. Norfloxacin appears to reduce the
following discharge into surface water bodies, potentially reducing their body size of collembolans and the quantity of eggs laid in laboratory
potential environmental impact [72]. simulation experiments on Petri dishes [87]. Antibiotic use may alter the
Parent chemicals or modified forms of pharmaceuticals are generally microbial balance in the intestine. The antibiotic triclosan (TCS), for
conjugated or hydrolyzed in wastewaters. Hydrolyzed derivatives can example, had a considerable impact on the gut microbiota of the isopod
lead to the formation of parent compounds at a later period, such as after Balloniscus selowii, and the changes were severe enough to obstruct
discharge into a receiving body or during sewage treatment, providing nutrient absorption [88]. Norfloxacin was found to disrupt the intestinal
another endogenous source of drug release into the environment [73]. microbiota of F. candida in a Petri dish system [89]. Variations in the
Carbamazepine, for example, is discharged as glucuronides, which may amount of toxicity in various culture systems, on the other hand,
act as a storage for the parent material, which will be released later [74]. contributed to the differences in the gut microbiota’s reactions to
5
norfloxacin. In addition, the intestinal microbiota includes host-related (half maximal effective concentration) in the range of 5000 to 10,000
microbiota as well as soil microbiota that is temporarily resident in the g/L after 96 h of exposure. However, none of the trials included had
gut [90]. It is generally understood that addition of norfloxacin to soil exposure times longer than 96 h. The present data was insufficient to
altered the soil microbiota, particularly Gram-negative bacteria [83]. To cover all probable impacts of this antibiotic on the environment due to
understand the impacts of pollution on soil animals, studies that the lack of ecotoxicity testing with longer exposure periods that may
differentiate between the soil and intestinal microbiota are required, cover several growth phases of these microalgae [109]. While harmful
and may serve as new potential bioindicators. effects were evaluated for a single trophic level of species, such studies
for complex combinations of organisms were relatively rare for variety
3.2. Ofloxacin (OFL) of chemicals [109]. To create more realistic circumstances and give
accurate information on the possible antagonistic and synergistic effects
Ofloxacin is a carboxylic acid of the fluorinated quinolone-type of medicines, toxicity assessments of drug combinations and long-term
antibiotic usually applied for the treatment of respiratory and urinary exposure tests should be undertaken [110]. However, there have been
tracts infections, conjunctivitis, otitis, tuberculosis because to its wide few published toxicity studies on the temporal development of the EC50,
spread distribution and genotoxic effects [91]. WHO ranked OFL has one despite the fact that it is predicted that as exposure duration increases,
of the critically important drugs for human health due to its application the EC50 value decreases [111]. Xiong et al. [112], found that the reverse
[92]. OFL has poor bio-degradability which results to its accumulation increasing exposure duration resulted to higher EC50. Nunes et al. [113],
into the aquatic environment for longer period of time [93]. OFL has also reported that at low CIP concentrations (0.013 mg/L), there was a
been found in wastewater at amount ranging from 0.005 to 31.7 g/L, substantial decrease in lipid peroxidation levels, whereas at high CIP
even after standard treatment [94]. Due to its persistency against bio concentrations (0.078 mg/L), there was a significant rise up to 0.013
logical degradation, OFL cannot be removed through conventional mg/L of CIP. The genotoxicity test showed a substantial rise in genetic
wastewater treatment plants [93], and thus subsequently escape to damage index. The ecologically relevant ciprofloxacin doses examined
ground water and river surface. Furthermore, because biosolids are had no significant effects on D. magna life-history parameters; never
reused for agricultural purposes, OFL has been classified as a very theless, oxidative stress and genotoxic damage scenarios were noticed at
dangerous substance for the aquatic environment [94]. In Daphnia the same levels of ciprofloxacin.
magna F3 (third generation clone) and F4 (fourth generation clone),
Ofloxacin at 200 g/L has shown to reduce the number of offsprings 3.4. Clofibric acid (CA)
during initial reproduction [95]. Sometimes, the detected concentra
tions in aquatic environment may be lowered than the effective level on Clofibric acid (CA) is an active metabolite of lipid regulators such as
aquatic lives, however due to existence of pollutants in multiple syner clofibrate, etofyllinoclofibrate, and etofibrate which is utilized to make
getic actions of these multi-pollutants can occur on aquatic lives. anti-neoplastic, anti-lipemic, anti-cholesteremic, and even herbicides
Esposito et al. [96], reported that the presence of OFL in water surface [114]. Despite its widespread usage, little research has been done on its
with residence time of 246 h and around 13,920 h in soils. OFL is a chiral toxicity and ecological effects. However, there have been indications
molecule and its enantiomers are optically active thus revealed its su that clofibric acid and its metabolites, even at low concentrations in the
perior antibacterial power. Al-Omar [97] also reported that 90% of the ecosystem, can cause environmental damage [115]. Clofibric acid is
dose of OFL is eliminated unaltered in the urine, with a concentration of pseudo-persistent in the environment, according to experts, and. It’s
306.1 ng/L [98]. In an Italian hospital of 900 beds and 2000 personnel, crucial to look at its toxicological (acute and chronic) effects on the
it was found that the hospital wastewater contain OFL in at high con ecosystem.
centration (19 μg/L) above the concentration detected for ciprofloxacin There have been several reports of acute toxicity from clofibric acid
(12 μg/L) [99]. and its metabolites. For 48 h, Clofibric acid ecotoxicity EC50 endpoint of
Daphnid and ceriodaphnid assays yielded >200 mg/L [116]. The authors
3.3. Ciprofloxacin (CIP) discovered that Daphnid 21-day NOEC for clofibrate was 64 times lower
than the ceriodaphnid 7-day NOEC value reported by Ref. [116].
Ciprofloxacin (CIP), a fluoroquinolone-family broad-spectrum anti Clofibric acid appears to be less harmful to the aquatic environment
biotic, is utilized in human and veterinary medicine all over the world than clofibrate. Ferrari et al. [116], also obtained EC50 values of 28.2
[100]. CIP is partially or/and non-metabolized in animals after delivery, mg/L in 24-h daphid toxicity test,. Clodacerans were shown to be un
therefore the original compound and its metabolites usually release affected by the presence of clofibric acid, which had an EC50 of over 200
during excretion into the other environmental compartments, such as mg/L. In a study on the acute toxicity of clofibric acid on bacteria,
water bodies [101]. Furthermore, conventional wastewater treatment daphids, ciliates, and fish eggs, the authors observed a toxicity value of
techniques such as activated sludge or up-flow anaerobic sludge blanket roughly 14 mg/L [117]. As a result, exposure to clofibric acid and its
reactors have limitations on CIP removal [102], which can result in the metabolites may have an immediate influence on the environment. The
release of active compounds into aquatic ecosystems at ng/L and g/L toxicity of clofibric acid on algae was shown to be not less than 14 mg/L
levels respectively [102]. Diniz et al. [103], reported up to 34 g/L of CIP in a study undertaken to determine its chronic toxicity [117,118].
in hospital wastewater, an indication that CIP is a recalcitrant molecule Furthermore, Ferrari et al. [116], also discovered that when a chronic
with great environmental stability. Furthermore, CIP concentrations of toxicity test was performed on rotifers, a NOEC value of 0.25 mg/L
310 g/L or higher were reported to limit bacteria growth in activated proved to be more sensitive, suggesting that Clofibric acid can have a
sludge aeration tanks [104]. greater impact on non-target organisms. According to Ferrari et al.
The presence of antimicrobials in water bodies contributed to evolve [116], chronic toxicity studies showed greater toxicity than acute
resistance of bacteria genes [105]. Antimicrobial residues in the aquatic toxicity testing. For C. dubia, the acute EC50/chronic NOEC ratio was
environment also have an impact on aquatic biota other than bacteria, calculated to be > 312 mg/L. C. dubia was found to be more sensitive
including fish, copepods, microalgae and macrophytes [105]. CIP has than P. subcapitata, B. calyciflorus, and D. rerio in chronic concen
been linked to change in antioxidant enzymes in exposed organisms tration–effect relationship tests, with P. subcapitata and D. rerio being the
[106], which have been linked to genotoxicity in bacteria (Salmonella least vulnerable.
thyphimurium) [107] and chronic toxicity in the microalgae, Raphidocelis A huge carp in India (Cirrhinus mrigala), the toxicity of Clofibric acid,
subcapitata, Chlamydomonas reinhardtii, Chlorella vulgaris, and Chlamy one of the most regularly identified medicines in the aquatic environ
domonas Mexicana [107]. Venancio et al. [108], studied the chronic ment was examined. Saravanan et al. [115], revealed that Indian carp
toxicity of CIP in Raphidocelis subcapitata, and the authors reported EC50 fingerlings were exposed to clofibric acid at concentrations of 1 g/L, 10
6
g/L, and 100 g/L for 96 h and 35 days, respectively. TSH levels were for 24 h at a fatal dose of 59.70 mg/L, and it was found that CBZ caused
observed to be lower at all doses of Clofibric Acid over the 96-h and changes in the activities of glutamate pyruvate transaminase, glutamate
35-day exposure periods (except in 1 and 10 g/L at the end of the 14th oxalocetate transaminase, and lactate dehydrogenase in numerous or
day and 1 g/L at the end of the 21st day) [115]. At 1 g/L and 100 g/L of gans [132].
Clofibric Acid exposure, T4 levels were shown to be lower after 96 h. The term “chronic effect” refers to an unfavorable impact of carba
During the 35-day exposure period, T4 levels were reduced at all Clofi mazepine that arises after a single or many exposures over a lengthy
bric Acid doses. T3 levels in the treatments were lower in fish exposed to period of time. This has been proven in several investigations. For
all doses of Clofibric Acid. These findings showed that the Clofibric Acid instance, Ferrari et al. [116], looked at the long-term effects of CBZ on
medication caused substantial alterations (P < 0.01) in C. mrigala thy the Ceridaphria dubia (micro crustacean) and found that chronic toxicity
roid hormone levels. Changes in these hormone levels might be was greater than acute toxicity. Almeida et al. [133], revealed that CBZ
employed as biomarkers for pharmacological medication monitoring in levels in Ruditapes philippinarum tissues increased throughout the
aquatic organisms [115]. exposure gradient. When the exposure concentration was increased, a
Clofibric acid, a derivative of clofibrate, has been a major cause of rise in CBZ in clam tissue was detected, reaching a peak of 6 ng/g fresh
concern due to its frequent occurrence in the environment [119] and weight at 9.00 μg/L. Almeida et al. [133], reported that after 28 days of
high societal demand. The first findings on the existence of clofibric acid exposure, the death rate was 5% for 0.03 μg/L, and 11% for 3.00 g/L,
in the environment were published in 1976 [120,121]. Garrison et al. whereas the mortality rate for 9.00 μg/L was zero. Contardo-Jara et al.
[121], discovered low concentration of clofibric acid in treated waste [134], measured CBZ accumulation in the Dreissena polymorpha (Zebra
water in the United States at (ng/L). Thereafter, in 1998, Quero-pastor mussel) after 4–7 days of exposure and found that the concentration of
found CA in surface water at values ranging from 0.049 to 0.066 mg/L CBZ ranges from 0.236 to 236 g/L and that CBZ accumulation increased
[120] and in drinking water at maximum concentrations of 270 ng/L with exposure time at all concentrations. Long-term exposure to CBZ has
[122]. In tests conducted in the United States, this chemical was also been linked to a variety of disorders, including antibiotic resistance in
discovered in lakes and rivers [120]. Further research also revealed human pathogens, carcinogenicity, genotoxicity, endocrine disruption,
possible presence of endocrine disrupting substances [123]. The pres allergic responses, and reproductive and developmental consequences
ence of pharmaceutical compounds in the environment pose serious risk [4]. Stevens-Johnson syndrome and its related disorders have been
to human health and other living things in general, according to some linked to CBZ consumption in Southeast Asian nations [135]. Samantha
studies, even at extremely low concentration levels [120]. Clofibric acid, [136], also linked the neuro-developmental abnormalities in the human
in particular, has a deleterious impact on the liver, resulting in gallstones embryo in the womb to CBZ exposure. Atkinson et al. [137], also re
[124]. ported that exposure to carbamazepine during pregnancy contributed
largely to fetal death and congenital malformations [131]. Also, the CBZ
3.5. Carbamazepine (CBZ) detected in ground and drinking water constitute additional risk embryo
and newborn through breast-feeding or intrauterine exposure. The in
Carbamazepine’s effectiveness has been highly commendable in the dicator parameters for the selected emerging micropollutants are sum
field of medicine for the treatment of many disorders such as depression, marized in Table 2.
epilepsy, and arrhythmia. However, due to its extensive usage, the
compound and its metabolite have been detected in water bodies in 4. Overview of treatment methods for hospital wastewater
concentrations ranging from ng/L to ug/L causing various adverse ef adopted in three continents
fects on aquatic species [125]. Carbamazepine’s ecotoxicology has been
studied by a number of scholars. For instance, Carbamazepine concen There are different techniques used in different nations for Hospital
trations ranged from 230 to 1110 ng/L in Shanghai’s sewage treatment wastewater treatment. Table 3 summarizes all of the techniques used,
facility, and 1090 ng/L in the Yangtze River, according to Chen et al., along with the citations. This will help the reader to understand some
[126]. Also, Liu et al. [127], reported 100% CBZ was identified in peculiarity based on the developmental status and regional factors of a
Nanjing rivers, between 0.05 and 1.6 ng/L concentration in the fish country.
bodies and 0.2 and 6.9 ng/L concentration in the water system. Simi Typically, hospital wastewater is released into the municipal sewer
larly, Xie et al. [128], reported 0.24–8.74 ng/L concentrations of CBZ system, where it mixes with other effluents before being treated in a
detected in Lake Taihu, China, with 32% found in biotic samples such as sewage treatment plant. This is a common practice in countries like
crucuian carp, common carp, and yellow catfish. As a result, given the South Africa, Australia, Thailand, Iran, Japan, Egypt, and India. Hospital
high levels of CBZ in the ecosystem, it is critical to assess its harmful wastewater, on the other hand, can be a substantial source of hazardous
effects, both acute and chronic. materials in the aquatic environment because wastewater are released
Acute impact is defined as a carbamazepine side effect that develops directly untreated into drainage, lakes, and rivers in countries like
after a single or repeated exposure within 24 h. Depending on the con Taiwan, Algeria, Vietnam, Bangladesh, Nepal, Pakistan, Congo, and
centration, this might be severe or minor. Chen et al. [126], observed 3% India,. According to Ashfaq et al. (2019), no hospital in Pakistan has
of Daphnia similis died after 4 days, indicating no acute effect based on established sufficient wastewater treatment facilities, regardless of its
the present exposure concentration level (that is, no concentration – size. In Taiwan, several hospitals release their wastewaters directly into
dependent for all concentrations when testing for Chitobiase in Daphnia surrounding rivers (illegally or legally) without prior treatment [138].
similis). When exposed to 100 g/L, the acute effect was observed to be Only 48% of the 70 state hospitals in Iran have wastewater treatment
concentration-dependent, with EC50 values of 3985.24 μg/L for 48 h, systems, while 52% did not and such hospitals dumped their wastewater
345.58 μg/L for 72 h, and 306.17 μg/L for 96 h. Chen et al. [126], into wells, 38% dumped it into the environment, and the rest dumped it
revealed that CBZ concentration of 1 g/L promoted reproduction and into the municipal wastewater system [14]. When the indicators of
phototactic behavior in Daphnia magna. Aromatic amino acids used as wastewater treatment systems are compared to the norms of Environ
biomarkers for sub-lethal CBZ exposure, altered energy metabolism, mental Departments, it is clear that these systems are inefficient, and in
according to Kovacevic et al., [129]. CBZ respiratory quotient value of view of the recent development, Hospital wastewater treatment systems
4.69 was similarly recorded by Ying et al. [130], suggesting danger of need improvement.
CBZ to aquatic species [131]. Other researchers, such as Ferrari et al. In Indonesia, 64% of hospitals released their wastewater directly into
[116], have noted relatively little acute toxicity on bacteria, infiltration well or water bodies while 36% have wastewater treatment
micro-crustaceans, algae, and fish, therefore not an immediate concern. plants [139]. Wastewater Treatment Plants in Hospitals often employ a
Another investigation was carried out on Cyprinus carpio (common carp) combination of chlorination and biological methods, with the discharges
7
Table 2
Indicator parameters for emerging micropollutants.
Indicators Norfloxacin Ofloxacin Ciprofloxacin Clofibric Acid Carbamazepine
Concentration in 6.8 μg/L 6.6 ng/L >1.0 μg/L 1.0 mg/L 8.74 ng/L
water
Concentration in soil 9.8 μg/L 0.3 mg/L 5.0 mg/g 5.0 mg/g 6.0 ng/g
Acute Toxicity EC50 of 400 mg in 12 h – – EC50 > 28.2 mg/L in 24 h –
Chronic toxicity EC50 of 800 mg in 28 days – EC50 after 96 h EC50 > 312 mg/L in 35 EC50 after 4 days
days
Metabolism Biliary excretion and Renal excretion. Renal excretion. Renal Renal excretion. Renal excretion.
excretion.
Biomarkers ≥0.4 mg/L after 4 and 7 days in gold 0.05 mg/L after 4 or 7 days in gold – – –
fish. fish.
be under threat. The direct or indirect discharge of untreated hospital

Table 3
wastewater into the environment has been ascribed to different abnor
Treatment scenario of hospital wastewater in different countries.
malities in aquatic organisms. Some of the treatment methods used in
Country Treatment References different country are shown in Table 3.
Algeria Direct release into the ecosystem [143]
Australia Co-treatment [14] 5. Analytical techniques for determination of micro-pollutants
Bangladesh Direct release into the ecosystem [144]
in hospital wastewater
China Specific treatment [145]
Congo Direct release into the ecosystem [146]
Egypt Co-treatment [147] Several analytical techniques have been applied for detection of
Ethiopia Direct release into the ecosystem [148] different concentration of emerging organic pollutants present in hos
India Co-treatment/Direct release into the ecosystem/ [149] pital wastewater ranging from spectrophotometry to advanced micro
specific treatment
Indonesia Direct release into the ecosystem/specific [139]
scopic method. This will help the reader to understand the merits and
treatment demerits of one analytical technique over the other and most suitable
Iran Specific treatment/co-treatment [150] among them all.
Iraq Specific treatment [151]
Nepal Direct release into the ecosystem [152]
Republic of Specific treatment [2] 5.1. Spectrophotometry
Korea
Taiwan Direct release into the ecosystem [153] Spectrophotometry is a branch of electromagnetic spectroscopy
Vietnam Direct release into the ecosystem [154]
concerned with the quantification of radiant energy transmitted or re
Japan Co-treatment [155]
Pakistan Direct release into the ecosystem [156] flected by a body as a function of wavelength [159]. The notion is
South Africa Co-treatment [157] straightforward, but calculating reflectance or transmittance necessi
Thailand Co-treatment [158] tates careful consideration of the measurement’s geometrical and
spectral circumstances. For decades, spectrophotometric equipment
have been utilized in laboratory, industrial and educational institution
frequently exceeding quality standards for typical treated wastewater
[160]. There are different types of spectrometry; general purpose
especially for phenol, lead, ammonia-free, free chlorine and
UV–Visible, high resolution UV–Visible, Scientific Grade High Sensi
ortho-phosphate. Low-quality discharges from hospital wastewater
tivity, Fourier Transform [161]. General purpose Pre-dispersive spec
treatment plants, contain hazardous pollutants (lead and phenol),
trophotometer designs are also common. This implies that the source
generated by a biological-chlorination process that are yet to be opti
released white light split into spectra and pass via the sample with its
mized [140]. In 2004, a research conducted in Kunming, a big city in
wavelength to the detector one at a time [159]. A benefit of this design is
China’s South West revealed that 36 out of 45 hospitals have wastewater
that the sample is exposed to significantly less light energy than in
disinfection equipment. In the same year, 50 hospitals in Wuhan,
post-dispersive systems. The fundamental drawback is that only one
China’s largest city in the Central Southern area had their wastewater
wavelength may be studied at a time, and spectra must be constructed
treatment facilities audited. It was also revealed that 46 hospitals had
from data points collected at various intervals [161]. Several
wastewater treatment facilities, with just around half of them fulfilling
micro-pollutants have been studied and detected using UV–Visible
the national discharge standard [141]. Most hospitals in Iraq have
spectrometer namely ciprofloxacin, ofloxacin, norfloxacin moxifloxacin
treatment plant, however not up to Iraqi requirements, particularly in
among others. Ciprofloxacin was analyzed as a pollutant and the con
terms of nutrient and pathogen elimination [140]. In nations like China,
centration was found to be 0.5–25.0 μg/L [162] while ofloxacin was
the Republic of Korea, and Indonesia, where hospital wastewater is
found to be 1.0–35.0 μg/L [98]. Norfloxacin and moxifloxacin were
handled on-site, the situation is more strict (specific treatment).
found to be in the range of 5–150 μg/L [163] and 2.65–230 μg/L [164]
Non-governmental organizations (NGOs) are actively using this method
respectively. Therefore, Spectrophotometry has different merit and
(that is, hydrated (slaked) lime (Ca(OH)2) coagulation/flocculation with
demerit; such as good sensitivity, simplicity in operation compared to
aluminum sulfate and disinfection) to assist manage human excreta in
other techniques for analyses while its detection index is single. How
various emergency contexts, such as Ebola and various infectious dis
ever, the technique has a poor colour material stability and high inter
ease epidemics in Philippines, West Africa, and Myanmar [142]. Table 3
ference [159].
represents different treatment scenario of hospital wastewater in
different countries. Some of these treatment approaches are
co-treatment, specific treatment and direct release into the ecosystem. 5.2. Gas chromatography
These are proof that there are still needs for advanced approach as
regards treatment of wastewater especially hospital wastewater which Gas chromatography is a chromatographic technique which involves
require separate treatment attention. Without successful treatment of mobile phase and a suitable gas used for separation of a given sample
hospital wastewater, aquatic organisms and human life will continue to such as crude substances [165]. In 1955, James and Martin developed a
classy form of gas chromatography with solid as the stationary phase or
8
liquid form while the mobile is in gaseous form. In the stationary phase, 5.4. High performance liquid chromatography (HPLC)
when a component is more soluble, it moves slowly across the column,
but when it is less soluble, it moves faster [165]. As a result, depending High performance Liquid Chromatography (HPLC) is an improved
on their partition co-efficient between the stationary phase and the form of column chromatography which is otherwise called high pressure
component of interest, the components in the sample mixture are liquid chromatography, and it is applied to separate lipid mixture via
divided into two groups. The nature of the stationary phase determines stationary phase filled column. This powerful tool is very fast, since it
how gas chromatography is classified: There are two forms of chroma required solvent to be forced via high pressures of up to 400 atm. It also
tography: gas-liquid chromatography and gas-solid chromatography required very small particles size for the package of column material
[166]. which results to a greater surface area for interaction between the
Gas–solid chromatography (GSC) refers to chromatography in which molecule and stationary phase for a better separation of the mixture
the stationary phase (adsorbent) is solid (GSC). Active carbon, silica, and components. Kirkland and Huber were the first to suggest high-
alumina [166]. In GSC, the separation principle is adsorption, it has a performance liquid chromatography (HPLC) [172]. In the 1970s, the
long column life, but the main disadvantage is the possibility of changes HPLC technology was developed based on the concept of column chro
in the component chemical composition present in the combination of matography under high pressure and involves pushing the mobile phase
sample [167]. Gas–liquid chromatography (GLC) is when liquid is the via packed column. In HPLC, the pressure mobile phase is at the top and
stationary phase of gas chromatography. A solid surface, such as a the stationary phase is at the bottom of the column. HPLC techniques are
polymer, is used to immobilize the liquid. GLC’s guiding principle is based on four approaches: chromatography mode, separation principles,
partition. Nowadays, GLC is frequently utilized in the form of a capillary scale of operation, and analytical types [172].
column. There are two types of HPLC categories: reverse and normal phases,
Gas chromatography has a number of advantages, including high based on the chromatographic mode. In normal phase HPLC, the polar
separation power for most complicated mixtures. The approach is components such as silica gel are in stationary phase while the non-polar
extremely sensitive, requiring only a minimal sample size for examina components are in mobile phase. In contrast to mixture of polar com
tion. It is equipped with a high-sensitivity detecting technology that is ponents, non-polar components of interest move swiftly and are eluted
precise and accurate. The operation is accomplished in a very short first with this approach because non-polar components have a lesser
amount of time and with excellent linearity [168]. The instrument cost is affinity for stationary phase [173]. Due to their higher affinity for the
relatively low, easy to handle and high durability and relatively suitable stationary phase, the polar components of interest present in the mixture
for routine analysis with high precision. There are still some short are retained in the column for longer period of time and eluted later than
comings such as: low Sensitivity. In most cases, the analysis often the non-polar components [174]. In reverse phase HPLC, the stationary
involve volatilization, and there’s a danger the sample will degrade phase and the mobile phase are normally non-polar and polar respec
[168]. The column cannot be utilized for biological sample analysis due tively. In this mode, the non-polar molecules are retained in the column,
to its high temperature. Gas chromatography has been applied in various after the polar components of the mixture are eluted. Most drugs are
field of research for gaseous samples. It is used to determine how many polar, and do not stay in the column for a longer period and thus quickly
organometallics are present in a given substance. It is also used to figure eluted [175].
out how much estrogen is in human body. Antituberculosis pharma Partition chromatography, adsorption chromatography, size exclu
ceuticals, antibiotics, anti-neoplastic agents, antiviral treatments, oint sion chromatography, ion exchange chromatography, and affinity
ments, anticonvulsants, and steroids are all routinely determined using chromatography are some of the most used HPLC processes based on the
GC [167]. Furthermore, it is also used to check the quality of dairy separation principle [175].
products. Pesticides in aquaculture products are determined using this On the basis of scale of operation, HPLC are classified into analytical
method. It is used to diagnose some disorders, such as cancer. It is used and preparative type. The specified material is analyzed in analytical
to identify drugs and alcohols in the bloodstream [167]. HPLC. However, sample recovery is somehow difficult. In preparative
HPLC, the sample mixtures are always collected through the fraction
5.3. Gas chromatography mass spectrometry (GC-MS) collector while the collectors are reused [173].
HPLC can be classified into two type base on analysis-type such as;
In chromatographic methods, coupling of mass spectrometry is not qualitative and quantitative HPLC. Qualitative HPLC is used to identify
only associated with gas chromatography but also with liquid chroma the qualities of the components of a sample combination during anal
tography [169]. GC-MS helps to determine the compounds present and ysis. Quantitative analysis is used in HPLC to determine how much of
to compare their concentrations. This can be achieved through these two each component of the sample mixture is present [176]. This analysis is
prerequisites: i. Determination of the individual compound by their carried out once the peaks have been detected and integrated [175]. The
identification of the mass spectrum and ii. Calculation of the abundance thickness of the stationary phase, particle size of the stationary phase
peaks corresponding to those compounds in each sample [170]. These packed in column, internal diameter of the column, flow rate of the
prerequisites are sometimes difficult and often resulted to waste of time mobile phase, length of the column, viscosity of the mobile phase, af
due to peaks co-elution within a chromatogram and shift of retention finity of the component of interest (analyte) with mobile phase, nature
time across samples. These two shortcomings can lead to mix of mass of the mobile phase, and staining of the component of interest (analyte)
spectra and complicate the identity and quantification of the compound with mobile phase are the most important components that affect the
[170]. Most traditional vendor software assess compounds based on HPLC technique efficiency [176].
peak area or height by picking m/z values typical for the specified HPLC has been widely used in the separation of alkaloids present in
component from total ion count (TIC), base peak chromatogram (BPC), plants and inorganic ions such as chloride, phosphate fluoride, bromide,
or extracted ion chromatogram (EIC) [170]. This technique is vulnerable nitrite, cadmium, magnesium, copper, lead, and zinc ions, detection of
to co-eluting compounds provided the contribution to the signal from intoxicants, poisons in human blood, and addictive drugs such as
other chemicals is not well managed. This can have a major impact on alcohol, cocaine, morphine, heroin, and opioid drugs, and identification
both quantitative and qualitative results [171]. Furthermore, the esti of illicit drugs [173]. It is also employed exclusively in forensic science
mation of baseline contributions is difficult, and may result to errors in for investigation, explosives analysis, lipid, steroids hormone, and bile
quantification. Majority of currently used methods rely on basic back acid identification [177]. Different techniques along with their merits
ground subtraction from a local baseline or a shoulder of a specific peak and demerits are listed in Table 4 while different analytical techniques
of interest especially when dealing with overlapping and/or co-eluting applied for the detection and quantification of pollutants in hospital
peaks [171]. wastewater is provided in Table 5.
9
Table 4 6.1. Physical techniques

Analytical Techniques, their Merits and Demerits.
Techniques Merits Demerits References The treatment of hospital wastewater involving combination of
coagulation/flocculation/precipitation with Al2(SO4)3 or FeCl3 or ap
Spectrophotometry Sensitivity: High and Detection index: [159]
Good single pears to be a viable option for the removal of lipophilic compounds like
Operation: simple and Colour material diclofenac from the liquid phase [186]. These methods however unable
easy stability: Poor to remove several hydrophilic pharmaceuticals such as iopromide,
Interference: High diazepam, carbamazepine, and antibiotics such as trimethoprim eryth
Gas chromatography Powerful separation Unstable heat or [167]
functioning high boiling point
romycin, roxythromycin, among others [187]. Suspended particles,
chromatographic substances is which can be detected up to three times higher quantities in hospital
column difficult to wastewater than in municipal sewage, can be removed effectively by
Optional detectors of analyze. flocculation/coagulation [188], thus preventing their accumulation on
specific purpose from Malodorous
primary and secondary sludge. Flotation appears to remove persistent
general purpose sample with
complex chemicals like carbamazepine (approximately 20%) [189].
components is not
suitable to detect 6.2. Biological techniques
since there is
certain selectivity
of substances
Due to the action of co-metabolic and metabolic mechanisms in these
Gas chromatography Detection range: Structural [169] systems, biological treatments are one of the most effective secondary
Mass Widely recognition of treatments barrier to most Pharmaceuticals [190]. The longer sludge
Spectrometry Strength: Strong similar retention time (>25–30 d) boost removal efficiencies, while some
Sensitivity: High compound: weak
chemicals have thresholds beyond certain limit [191]. Membrane bio
Anti-interference: Able Professional
needed for logical reactors and conventional activated sludge effluents have equal
complex removal rates for basic pharmaceutical compounds like ibuprofen [192].
operation For several substances, membrane biological reactors performed better
High performance No limitation by Long analysis time [172] than traditional activated sludge, by providing a 30–50% higher
Liquid sample volatility High cost
Chromatography Determining organic
removal rate in some circumstances. Furthermore, membrane biological
compound with high reactors have regularly demonstrated a 40–65% improvement in the
boiling point, high elimination of certain chemicals that are resistant to standard activated
relative molecular sludge treatment such as; indomethacin, diclofenac, mefenamic acid,
weight and poor
and gemfibrozil among others [19]. There is no link between the
thermal stability
Analyzing at a lower chemical structure of pharmaceuticals and the rate of elimination. For
temperature most chemicals, however, the variation range in removal rate exhibited
in membrane biological reactors is limited, whereas bigger fluctuations
are recorded in traditional activated sludge [193]. The superiority of
Table 5 membrane biological reactor processes has also been claimed in term of
Different analytical techniques applied for detection and quantification of pol pathogenic microorganisms elimination, including various viruses [5].
lutants in hospital wastewater. A biological reactor’s performance can be improved by separating it into
reactor cascades [194]. In wastewater treatment plants with longer
Analytical Techniques Pollutants Concentration References
(μg/L) sludge retention times, nitrifying bacteria play an important role of
pharmaceuticals biodegradation [195].
UV–Visible Ciprofloxacin 0.5–25.0 [162]
Ofloxacin 1.0–35.0 [98]
Norfloxacin 5–150 [163] 6.3. Adsorption techniques
Moxifloxacin 2.65–230.0 [178]
Gas chromatography mass 5-Fluorouracil 92.00 [179] Adsorption technology is one of the most simple and cost effective
spectrometry Cyclophospamide 0.019–4.486 [180]
Ifosfamide 0.048 [181]
methods of decontaminating wastewater through the removal of con
Metoprolol 17–110 [182] taminants or pollutants in the aqueous matrix based on adsorbate-
Amphetamines 0.1–0.4 [183] adsorbent interaction [196]. The pollutants are the absorbate while
High performance liquid Carbamazepine 0.463 [163] the absorbent is the catalytic surface used [42]. The most known ad
chromatography Clofibric acid 0.772 [184]
sorbents are agricultural wastes, activated carbon, silica gel, and cotton
Diclofenac 0.05 [163]
Caffeine 5.65 [163] fibres [197], which have been used for the removal of different pollut
Ultra high performance Metformin 1.31 [185] ants such as micro-pollutants, endocrine disruptors, herbicides even at
liquid chromatography Diclofenac 0.59 [185] low concentrations from wastewater, [198–201]. Two primary ap
Ibuprofen 0.62 [185] proaches, static and dynamic methods, are used in the adsorption pro
Paracetamol 137.98 [99]
cess. Finely split adsorbents are agitated with water in the static method,
Acetaminophen 2.66 [185]
Caffeine 35.29 [99] and then separated by decantation or filtration. In the dynamic process,
Atenolol 0.20 [185] wastewater flows continuously across a fixed, mobile, or fluidized
adsorbent layer [202]. The majority of chemical procedures used in
hospital wastewater treatment generate a substantial amount of sludge,
6. Methods of treatment of hospital wastewater
which must be disposed of further. When used on dilute wastewater with
lower levels of micropollutants, these procedures are either inefficient or
Different conventional and advanced methods mostly applied for the
ineffective, and they necessitate a high level of skill.
treatment of hospital wastewater are explained in the next section.
6.3.1. Principles of adsorption techniques
Adsorption is the accumulation of a liquid or gas or solute (adsor
bates) on the surface of a solid (adsorbent) over time while absorption
10
occurs when a substance diffuse into a liquid or solid [203]. The both existence of weak forces of attraction (Van-der Waals) between the
terms encompasses the same process. While desorption is the reverse adsorbate attach to the surface of the adsorbent. It is also responsible for
process of the both terms [204]. Surface energy, which is related to the non-ideal behavior of actual gases. In chemisorption, there is exis
surface tension, causes adsorption. In a material, the constituent atoms’ tence of strong force of attraction (covalent or ionic types) between the
bond requirements, such as ionic, covalent, or metallic, are filled up, but adsorbate and the adsorbent’s surface [205].
bond deficiency occurs on the surface since they are completely sur
rounded by other atoms. As a result, the type of the bonding is deter 6.3.2. Adsorption mechanism of the five selected emerging micro-pollutants
mined by the nature of the participating species, and the adsorption The mechanism of adsorption of the selected emerging micro-
process is divided into physisorption and chemisorption [125]. Phys pollutants from aqueous media has been linked to several factors. So
isorption, also known as physical adsorption, is a kind of adsorption with lution chemistry is the main factor upon which adsorption mechanism is
Table 6
Adsorption mechanism of five selected emerging micro-pollutants with their adsorption capacity or percentage removal by different nano-adsorbents.
Emerging Nano-absorbent Experimental conditions pHpzc Adsorption Mechanism References
micropollutant capacity/
pH Contact Adsorbent Temperature
percentage
Time (h) dose (g/L) (◦ C)
removal
Ciprofloxacin. Graphene oxide/ 2.0 128 0.3 25 – 100.00 mg/g π-π interaction [208]
pKa = 6.09 sodium alginate
Bentonite-chitosan – 10 1.5 30 6.2 39.06 mg/g Ion-exchange [209]
Biochar from tea leaves 6.0 24 1.3 30 3.1 238.1 mg/g π-π interaction, H-bond, [210]
Electrostatic interaction
Magnetic N-doped 7.0 12 0.04 25 3.6 1564 mg/g π-π interaction, H-bond, [211]
porous carbon Hydrophobic interaction,
Fe2O4/graphene 6.0 72 1.0 25 6.3 283.4 mg/g Hydrophobic interaction [212]
oxide/Biochar
Activated carbon from 6.0 1.5 3.0 30 6.5 73.64 mg/g Intraparticle diffusion [213]
hazelnut
Modified hydrogel 8.0 12 0.25 20 8.3 154.9 mg/g H-bond, Hydrophobic [214]
beads interaction
Cationic flax noil 7.0 10 0.1 – 6.32 238.7 mg/g Electrostatic interaction [215]
cellulose
Activated and znO 4.0 24 0.2 40 3.4 449.4 mg/g Electrostatic interaction, [216]
doped camphor leaves π-π interaction, H-bond,
biochar Hydrophobic interaction
Ordered carbon 6.0 24 0.03 25 8.8 233.4 mg/g Hydrophobic interaction [217]
Activated carbon from 6.0 24 0.03 25 8.5 362.9 mg/g Hydrophobic interaction [217]
bamboo
Carbamazepine Magnetic activated 8.1 24 0.03 25 6.0 68.00 mg/g Electrostatic interaction [218]
carbon
pKa = 13.9 Hexagonal mesoporous 5.0 4 2.0 25 5.5 41.87 mg/g Electrostatic interaction, [219]
silicate H-bond.
Bentonite 3.0 – – 25 – 25.57 Electrostatic interaction [125]
MOF – 24 0.1 25 9.0 – Hydrophobic interaction [220]
MOF UiO-67 5.0 24 0.1 25 – 82.64 mg/g Hydrophobic interaction, [221]
π-π interaction
CuO/Cu2O/Cu-biochar – 24 2.0 25 9.5 Hydrogen-bonding, π-π [222]
interaction
Smectite 7.00 24 5.0 23 – π-π interaction, Hydrogen- [223]
bonding.
Zero-valent iron/Cu 5.0 1.5 0.2 – 5.0 26.15 mg/g; 95% Hydrogen-bonding, π-π [224]
nanoparticle interaction
Graphene oxide 2.0 2.0 1.0 25 4.87 99% π-π interaction, Hydrogen- [225]
nanoplatelets bonding.
Montnorillonite 6.0 24 1.5 25 – 97% Electrostatic interaction [226]
Nanoclay
Clofibric acid MOF (MIL-101) 4.0 12 0.1 25 – 92.1 mg/g Electrostatic interaction [227]
pKa = 3.18 MOF (MIL-100-Fe) 4.0 12 1.0 25 – 88.0 mg/g Electrostatic interaction [227]
Graphene oxide 11.0 2 1.0 25 3.9 994 mg/g π-π interaction [228]
Nofloxacin pKa Polydopamine 6.0 1.5 0.5 35 6.3 307 mg/g Electrostatic interaction, [229]
6.34 microsphere H-bond, π-π interaction
MOF (UiO-66-NH2) 8.0 6 0.1 25 6.2 222.5 mg/g π-π interaction, [230]
Microplastics 5.0 54 0.005 25 – 41.2% Polar-polar interaction, [231]
van-der-waal interaction,
π-π interaction, H-bonding.
Modified thermal – – 0.04 25 – 88.53% Covalent bond [232]
activated kaolin
Ofloxacin MOF (ZIF-8) 9.0 – 0.2 25 – 194.9 mg/g H-bond, Electrostatic [233]
pKa = 5.97 interaction, complexation
of unsaturated metal
Modified thermal – 4.2 0.04 25 – 91.46% Covalent bond [232]
activated kaolin
Calcined verdo-lodo 8.25 24 1.2 25 2.7 160.81 mg/g Electrostatic [234]
bentonite clay
11
dependent [206]. Therefore, for researchers to gain more insight on the ozone dose varies from 5 to 15 mg/L, with a contact time of 15–30 min
solution chemistry and how its affect adsorption mechanism, there is [242]. In general, > 90% of personal care and pharmaceutical products
need for further information on solution pH, adsorbent point of zero are removed under these conditions. The availability of particulate
charge (pHpzc) and the pKa of the adorbate. Considering the pKa of the matters at monitored amounts in the secondary effluent has no effect on
selected micro-pollutants as indicated in Table 6, it can be observed that the removal efficiency of soluble chemicals with high ozone reaction
the pKa1 of norfloxacin, ofloxacin, ciprofloxacin, clofibric acid and rates [243]. Fig. 1 summarized different methods of treatment with their
carbamazepine are 6.34, 5.97, 6.09, 3.18 and 13.9 respectively [90,125, merits and demerits.
184,206,207]. In combining these alongside with kinetic, isotherm, and Of all the treatment methods of hospital wastewater, advanced
thermodynamic models and spectroscopy analysis such as XPS, XRD and oxidation processes based on free radical mechanism have been widely
FTIR, the mechanism of adsorption of these selected emerging utilized to effectively decompose toxic recalcitrant emerging micro
micro-pollutants as mentioned in Table 6 can be properly explained. pollutants into harmless species. In recent times, researchers have
During adsorption process (Table 6), there are usually multi- shown that combined treatment approach for hospital wastewater are
mechanisms which can be identified in systematic ways. Thermody more feasible, economical and offer greater efficacy than a single
namic modeling determines adsorption mechanism through identifica advanced oxidation processes based on the synergetic effects between
tion of types of interactions such as; physisorption and chemisorptions the two methods [244]. The enhanced production of highly reactive
which is based on the magnitude of ΔG◦ . When eluents (such as; organic molecular species in the combined system within short period of time
solvent or distilled water) are effective, It usually implies the existence contributed to its overall efficiency [164]. This review focused on the
of a physical mechanism. Chemical adsorption is demonstrated by the chemistry of photocatalytic and photo-fenton technology.
efficiency of strong acids and/or bases. For further clarification, there is
always a need to consider the isotherm and kinetic models based on the 6.4.1. Photocatalytic and photo-fenton processes
best-fit assumed. The spectroscopic analysis also revealed the specific The principle of photocatalytic reaction is based on excitation of a
functional group and location onto which the interaction occurs. This is catalyst through the application of light such as visible or ultra-violet
especially crucial when it comes to the identification of the chemical light [18]. Generation of free radicals produced during photon action
bonds that cause chemical or physical interaction. The solution chem would lead to oxidation or breaking down of adsorbed compounds on
istry (pH, pKa, and pHpzc) is critical for the determination of chemical the catalyst surface [245]. The photocatalyst such as titanium oxide,
interactions between the adsorbate and adsorbent under different pH zinc oxide, tungsten trioxide, cadmium sulphide, silicon (IV) oxide and
regimes. It has been reported that the adsorption pHpzc and optimum copper oxide [205] converts chemical energy to photon energy via
pH controls the mechanism uptake. Therefore, the adsorbent-adsorbate reduction-oxidation reaction. This causes the activation of nano
interactions are affected by the pH of the solution. particles, leading to excitation of electrons from the valence band to
From Table 6, in norfloxacin, ofloxacin, carbamazepine, clofibric conduction band and generation of electron-hole pairs. This further re
acid and ciprofloxacin, At pKa1, the carbonyl group is deprotonated, acts with water and produce highly reactive hydroxyl radicals that
while at pKa2, the amine group is protonated [235]. These selectively convert organic compounds into harmless species [246]. The
micro-pollutants can exist as a cation, anion and zwitterions. At this degradation process is begun by oxidants such as OHo, which are
point, the adsorbent point of zero charge (pHzc) comes into play; when directly created by photolysis of water molecules adsorbed on the
the adsorbent surface has a net negative surface charge, absorption photocatalyst’s active site (see Fig. 2). Furthermore, the photo-fenton
could occur via cation exchange with the protonated amine group. In reaction has multiple stages depending on their participation in free
teractions with deprotonated carboxylic groups are complicated for radical reactions: generation of active oxygen with the presence of
those with a net positive surface charge [236]. It was observed that the species that initiates the oxidation, active oxygen containing species
major mechanism in these selected micro-pollutants are; electrostatic transformation, and transformation reaction of oxygen species with
interactions, π-π (dispersive) interactions, H-bonds, hydrophobic con organic compound and finally intermediate reaction termination. The
tacts, and pore diffusion because of their low solubility, and they tend to photo-generated ferrous ions enter Fenton reaction generate supple
be adsorbed in hydrophobic interactions [235]. The electrostatic inter mental hydroxyl radicals. Consequently, the oxidation rate of
action (acceptor-donor) attraction resulted when the adsorbate is pro photo-Fenton is accelerated compared to Fenton process [247]. In
tonated and persists in its ionic state (pH > pKa) based on the comparison to the Fenton reaction, the photo-Fenton reaction has a
adsorbate’s ionic charge and the adsorbent’s net surface charge. The significantly lower total iron usage and sludge production [248].
5.00–9.00 pH range has limited solubility because the adsorbate is Furthermore, photo-Fenton via solar or UV light has been shown to have
electrostatically neutral and exists as a zwitterion. The attraction or a considerable impact on microorganism inactivation in polluted water
repulsion between molecules with opposing charge is known as elec bodies [249]. However, the process is dependent on the nature of
trostatic interaction [237]. Electrostatic interaction would promote microorganism present [250] and the nature of water under treatment
uptake if the adsorbate-adsorbent contact is attractive. They must have [251]. In a study, it was found that spores of F. solani was more resistant
an opposing charge to the adsorbent’s net surface charge in order to to solar treatment than the vegetative cells of E. coli [252]. Hydroxyl
provide an attracting force. Electrostatic interactions are most common radicals with 2.80 V oxidation potential degraded refractory substances
when the adsorbent has a net negative surface charge in the pH range of such as chlorinated and phenolic compounds [253].
1–5.59. Fig. 2 gives the graphic illustration of photocatalytic and photo-
fenton mechanisms while Table 7 summarizes pervious research
6.4. Chemical techniques finding involving application of photo-fenton and photocatalytic for the
degradation of emerging micropollutants in aqueous solution. It was
Advanced oxidation processes based on ozone (O3/UV, and O3/ noted that there are few hybrid photo advanced oxidation processes
H2O2), Fenton-type reactions, and photochemical AOPs have been found (that is, photo-fenton and photocatalysis). Therefore, it is recommended
to be more efficient than ozonation and adsorption alone [238,239]. that hybrid advanced oxidation processes should be acquired for effi
Several nanomaterials specifically metal and metal oxides [197] have cient degradation of hospital wastewater since hospital wastewater is a
been employed for wastewater treatment without high efficiency. AOPs multi-micro-pollutants wastewater.
are usually employed for the treatment of recalcitrant compounds due to Table 7 shows that most studies used simulated solution of these
increase production of radicals (that is, hydroxyl) and photon-initiated emerging micro-pollutants and not real environmental wastewater,
breaking of carbon-halogen bonds [240,241]. Depending on the where the pollutants exist as mixture. The performance of each tech
Chemical Oxygen Demand (COD) in the wastewater, the typically used nology was experimental conditions dependent. Again, individual
12
Fig. 1. Different methods of treatment of hopsital wastewater.
intermediates D, E, implying that products B, C, and D, E may be

degraded in distinct ways. Furthermore, when compared to D, E, the
decomposition of A to B, C occurred much faster and across a much
wider range, implying that the degradation pathways of B and C should
be preferred for CIP degradation over GMC-TiO2 [276].
The intermediate A was likewise formed at first for the Degussa-P25
system, just as it was for the GMC-TiO2 system. However, it was
discovered that the amount of intermediate B-E produced, regardless of
the fluctuation ranges or the time necessary to reach peak, was signifi
cantly different from that of the GMC-TiO2 system; in particular, the
amount of intermediate E produced was extremely considerable [277].
This shows that the degradation pathways of CIP in the presence of TiO2
alone and GMC-TiO2 nanocatalyst differ. The CIP degradation inter
mediate byproducts via photodegradation route are presented in Fig. 3.
It was found that the mechanism of degradation of CIP followed hy
Fig. 2. Schematic representation of semiconductor photocatalytic mecha droxylation, dihydroxylation, and double dihydroxylation.
nism [254].
6.4.2.2. Degradation mechanism of norfloxacin. The degradation of
advanced oxidation process employed produced high efficiency within norfloxacin (NOR) degradation often occur through the following
short-period of time, though this should not be taken as indication of pathways Piperazine ring transformation, dehydroxylation, defluorina
good performance because simulated solution that did not contain tion, and decarboxylation [278]. The molecular ions, as well as mass
radical scavengers and other pollutants was used. Their inefficiencies to fragment ions, were detected by MS spectra based on the HPLC-MS
degrade organic pollutants in real environmental wastewater limit their analysis. Fig. 4 depicts the proposed NOR degradation routes. During
full scale industrial applications. the photocatalytic reaction, two main degradation pathways: hydrox
ylation (route 1) and piperazinyl ring cleavage (pathway 2), were pre
6.4.2. Degradation mechanism of the selected emerging micro-pollutants dicted according to the intermediate determination (pathway 2). The F
based on photocatalytic technology atom was hydroxylated immediately by ⋅OH in pathway 1, resulting in
This section addressed degradation of the five selected emerging the hydrolated-NOR intermediate (m/z = 317) [279]. Following ben
micro-pollutants (norfloxacin, ofloxacin, ciprofloxacin, clofibric acid zene ring opening of NOR2 and hydroxylation to generate NOR4 (m/z =
and carbamazepine). The degradations pathways are very complex 181) after the loss of C4NH6, piperazine ring clavation (NOR2; m/z =
which lead to generation of several intermediates that are even more 249) [279]. NOR2 further undergo decarboxylation to yield NOR5 (m/z
toxic and exert greater environmental impacts than the parent com = 175) through continual ⋅OH oxidation [279]. The quinoline ring
pound. Different analytical tools (GC-MS and HPLC-MS) were used to cleavage of NOR5 and the loss of functional groups –NH2 and –CH3 were
determine the intermediates and possible degradation pathways. responsible for the formation of NOR6 (m/z = 147). NOR7 (m/z = 113)
was formed from NOR6 through decarboxylation and hydroxylation
6.4.2.1. Degradation mechanism of ciprofloxacin. Fig. 3 shows the profile processes [280]. In pathway 2, ⋅OH oxidation gave rise to decarboxyl
of six intermediates identified during the photodegradation of cipro ation and piperazine ring breakage of NOR, resulting in the formation of
floxacin with the following molecular fragment ions at m/z of 348, 318, NOR3 (m/z = 227). The prominent peaks in the MS spectra of NOR2 and
274, 306, and 279 [275]. Comparing the profile of ciprofloxacin with its NOR3 imply that the piperazine ring transition was most likely a sig
intermediates, it was found that A was the first intermediate to form nificant factor for NOR degradation pathway [279]. Further minerali
during ciprofloxacin degradation, and the remaining four intermediates zation of the intermediates usually lead to the formation of low
(B-E) appeared gradually based on their polarity with compound A molecular organics such as CO2, H2O, F− , and NO−3 as inorganic products
during the photodegradation in the presence of graphitized mesoporous [89].
carbon (GMC)-TiO2 nanocatalyst [276]. Despite the fact that the four
intermediates B to E had a similar characteristics, it was observed that 6.4.2.3. Degradation mechanism of ofloxacin. The Transformation
the retention time differ and that distinguished intermediates B, C from Products (TPs) of Ofloxacin (OFL) were identified and demonstrated
13
Table 7
Emerging micropollutants degradation by either Photocatalytic or photo-Fenton, Photocatalytic-adsorption and photo-Fenton-adsorption processes.
References Treatment Nanomaterial Micro-pollutants Research Findings
Techniques
Sponza and Photocatalysis Nano-GO/M Ofloxacin COD (88%), TSS (82%), TKN (95%), 97% removal, at pH 7.8, after 60 min at UV
Alicanoglu power of 300 W.
[255]
Perini et al. [256], Photo-Fenton Fe2+ Ciprofloxacin 80–95% removal, iron of 0.56 mg/L, pH 7.4, H2O2 of 17 mg/L, initial
concentration 200 μg/L in 90 min.
Photo-Fenton Fe2+ Amoxicillin 80–95% removal, iron of 0.56 mg/L, pH 7.4, H2O2 of 17 mg/L, initial
3+
Photo-Fenton Fe Sulfathiazole 80–95% removal, iron of 0.56 mg/L, pH 7.4, H2O2 of 17 mg/L, initial
2+
Photo-Fenton Fe Sulfamethazine 80–95% removal, iron of 0.56 mg/L, pH 7.4, H2O2 of 17 mg/L, initial
Liu et al. [257], Adsorption- TiO2/Zeolite Sulfadiazine (SDZ) 90% of SDZ was removed within 120 min of both adsorption and degradation by
photocatalysis TiO2/zeolite dosage of 1 g/L at neutral pH
Chinnaiyan et al. Photocatalysis TiO2 Amoxicillin trihydrate At pH 7.6, dosage of 563 mg/L, reaction duration of 150 min, and a starting
[258], concentration of 10 mg/L, 90% elimination is achieved.
Photocatalysis TiO2 Metformin HCl At pH 7.6, dosage of 563 mg/L, reaction duration of 150 min, and a starting
concentration of 10 mg/L, 90% elimination is achieved.
Tri et al. [259], Photocatalysis Ag-doped g-C3N4 Tetracycline 96.8% removal, fir 120 min, under solar light condition
Konstas et al. Photocatalysis TiO2CN Venlafaxine 70% removal, in 90 min.
[260],
Ghenaatgar et al. Photocatalysis ZrO2/WO3 Dexamethasone 100% removal, initial concentration of 5 mg/L, pH 3, Dose of WO3 and ZrO2 to
[261], be 500 and 1500 mg/L respectively.
Beheshti et al. Photocatalysis TiO2 Sulfamethoxazole 61.28% removal, dosage of 500 mg/L, pH 4.
[262],
Photocatalysis WO3 Sulfamethoxazole 43.3% removal, dosage of 750 mg/L, pH 3.
Serna-Galvis et al. Photo-Fenton Fe(II) Levofloxacin 54% removal, after 90 min, 1 mg/L of Fe(II), 10 mg/L of H2O2, pH 6.5, 500 W/
[263], m2
Sun et al. [264], Photo-Fenton α-FeOOH Sulfadiazine 100% removal, within 60 min, initial concentration of sulfadiazine of 12 mg/L,
H2O2 of 10 mmol/L, UV intensity of 100 μW/cm2.
2+
Della-Flora et al. Photo-Fenton Fe Flutamide 58% removal, for 40 min, dose of 5 mg/L, 150 mg/L of H2O2.
[265],
Serna-Galvis et al. Photo-Fenton Fe(II) Oxacillin 15% removal, after 90 min, 1 mg/L of Fe(II), 10 mg/L of H2O2, pH 6.5, 500 W/
[263], m2
Vieira et al. [266], Photocatalysis Fe◦ Diclofenac 100% removal, 98% COD, dose of 0.36 g/L, for 60 min, at MW power of 780 W
Photocatalysis Fe◦ Ibuprofen 100% removal, 98% COD, dose of 0.36 g/L, for 60 min, at MW power of 780 W
Wu et al. [267], Adsorption- La/Mg–Al with the Tetracycline 99.87% of TCH was removed within 110 min and reduced to 95.88% after five
photocatalysis La2O3 hydrochloride (TCH) cycle times.
Della-Flora et al. Photo-Fenton Fe(II) Fluconazole 80% removal, initial concentration of 500 μg/L, H2O2 of 100 mg/L, time of 10
[268], min
Photo-Fenton Fe(II) Flutamide 99% removal, initial concentration of 500 μg/L, H2O2 of 100 mg/L, time of 10
min
Photo-Fenton Fe(II) Furosemide 99% removal, initial concentration of 500 μg/L, H2O2 of 100 mg/L, time of 10
min
Photo-Fenton Fe(II) Chloramphenicol 99% removal, initial concentration of 500 μg/L, H2O2 of 100 mg/L, time of 10
min
Lumbaque et al. Photo-Fenton Fe3+-EDDS Dipyrone Above 77% removal, 500 μg/L of dipyrone, 230 mg/L of H2O2, at circumneutral
[269], pH.
Photo-Fenton Fe3+-EDDS Diazepam Above 77% removal, 500 μg/L of Diazepam, 230 mg/L of H2O2, at circumneutral
pH
Photo-Fenton Fe3+-EDDS Fluoxetine Above 77% removal, 500 μg/L of Fluoxetine, 230 mg/L of H2O2, at
circumneutral pH
Photo-Fenton Fe3+-EDDS Paracetamol Above 77% removal, 500 μg/L of Paracetamol, 230 mg/L of H2O2, at
circumneutral pH
Photo-Fenton Fe3+-EDDS Propranolol Above 77% removal, 500 μg/L of Propranolol, 230 mg/L of H2O2, at
circumneutral pH
Photo-Fenton Fe3+-EDDS Progesterone Above 77% removal, 500 μg/L of Progesterone, 230 mg/L of H2O2, at
circumneutral pH
Wu et al. [270], Adsorption-Photo- L-MIL-53(Fe, Mn, Cu) Ciprofloxacin (CIP) 15.2 and 2.49 times increase in reaction rate constant of CIP for L-MIL-53(Fe,
fenton. Mn) and L-MIL-53(Fe, Cu) respectively.
Abbasi et al. Adsorption- GO-CeO2 Doxorubicin (DOX) 97% of DOX was removed within 360 min. The pH of the DOX solution widely
[271], photocatalysis affected the removal process; neutral and alkaline conditions of pH supported
the degradation process
Chen et al. [272], Adsorption- MIL-53(Fe, Al) Tetracycline 71.39% and 81.82% of tetracycline were removed by MIL-53(Fe) and MIL-53
photocatalysis (Al). within 50 min.
Xu et al. [273], Adsorption- β-Bi2O3/ZrO2 Levofloxacin (LVF) 92.7% OF LVF was removed with 100 min.
photocalaysis
Adsorption- β-Bi2O3/ZrO2 Tetracycline 90.1% of TC was removed within 100 min.
photocalaysis hydrochloride (TC)
Adsorption- β-Bi2O3/ZrO2 Oxytetracycline 91.2% of OTC was removed within 100 min.
photocalaysis hydrochloride (OTC).
Chen et al. [207], Adsorption-photo- LaFeO3/Lignin- Ofloxacin 95.6% of Ofloxacin was removed with 75 min.
fenton biochar
Liu et al. [274], Adsorption – Cu–Fe bi-metal/g- Tetracycline Tetracycline removal efficiency over a wide pH range.
Photo-Fenton. C3N4 Nanosheets.
14
Fig. 3. The Degradation Pathway for Ciprofloxacin through photocatalysis [276].
using HPLC-ESI-Q-TOF-MS with the value of mass/charge (m/z) and LC/ 6.4.2.4. Degradation mechanism of clofibric acid (CA). The photo
MS patterns. Fig. 5 depicts the OFL transformation route and associated catalytic degradation route of CA are shown in Fig. 6 based on proposed
TPs. The attack of oxidative species such as hydroxyl radicals on the C–C molecular structures of the by-products. There are different pathways
bond of OFL, resulted in the formation of acetaldehyde groups in TP1. for photodegradation mechanism of clofibric acid [120]. Pathway 1
Due to the instability of the aldehyde derivative, it was further subjected followed the e− reductive mechanism, which involved dechlorination of
to additional oxidation, culminating in the production of TP2 [281]. C3–Cl. The radical’s 2-methyl-2-phenoxypropanoic acid was generated,
Following that, the hydrogenation reaction was the most common way which were then oxidized by HO⋅ to produce P1 [282]. The reaction of
for TP2 to become TP3. The development of TP8 from TP2 was caused 2-methyl-2-phenoxypropanoic acid radicals with diaquooxonium ions
by a C–N bond rupture. The production of TP9 was caused by the and hydrated electrons led to the formation of 2-methyl-2-phenoxypro
decarboxylation process. TP8 could be derived directly from OFL as an panoic acid radicals. P3 is formed as a result of this. As a result, the
essential intermediary [281]. Decarboxylation was also used to create aldehyde and benzene predictions were accurate [282].
TP4. The species that are active •O−2 is included. h+ attacked the The ipso-substitution reaction was responsible for Pathway 2, in
piperazinyl substituent in OFL, resulting into complete demethylation which the aromatic hydrogen compound’s ipso C was attacked by HO⋅,
process and formation of TP5 [207]. TP5 was then subjected to a series resulting in hydroxytative carbon-centered radicals. A series of P2 was
of tests. Due to h+ attack, the decarboxylation step occurred, and the generated during O-dealkylation processes when the chain was cleaved.
product was converted into TP6. After that, with a subsequent radical The electrophilic adduct process by HO⋅ attack, resulted in the creation
attack of TP6, TP7 was formed [281]. The formation was aided by of mono- and multihydroxylation byproducts, illustrated by Pathway 3.
demethylation and hydroxylation. The TP11 was obtained as a result of P4 was formed when HO⋅ attacked at C2. P5 was formed after additional
the demethylation procedure and majority of the observed in oxidation of P2. When HO⋅ attacked C12 via demethylation and decar
termediates were later oxidized and eventually mineralized into CO2 boxylation, transitory states of HO⋅ adduct radicals were generated,
and H2O [281]. resulting in the creation of HO⋅ adduct radicals [282]. Additionally,
15
Fig. 4. Degradation pathway of Norfloxacin through photocatalysis [279].
Fig. 5. Degradation pathway of Ofloxacin [281].
16
Fig. 6. Degradation pathway of Clofibric acid through photocatalysis [282].
processing of the hydroxylated by-product produced stable oxidation chloro-compounds such as; P7–P9.
by-product (P10). 1O2 hitting the aromatic C atom started Pathway 4 as
a result of the reduced FED2HOMO + FED2LUMO(1O2/dioxetane mechanism) 6.4.2.5. Degradation mechanism of carbamazepine. Fig. 7 shows time
value. Endoperoxides are formed when 1O2 reacted with CA at C3. Aside course profiles of HPLC-SIR-MS spectra for carbamazepine degradation
from that, 1O2 stayed on the stimulated surface longer and increased the under UV light by BPO-180-72. The peak area of carbamazepine rapidly
interaction with the substrate on the surface [282]. As a result, the reduced as the irradiation period increased, but new distinctive peaks
aldehyde and acid combined because of the endoperoxide, a chloride developed indicate conversion of carbamazepine into different trans
byproduct (P6) was then produced. Some researchers have reported formation products [283]. For instance, ten major intermediates were
similar aldehyde and carboxylic acid production mechanisms [282]. CA with mass to charge ratio (m/z) at 253.1, 149.0, 259.1, 275.0, 253.1,
and its byproducts could further reduced to generate small molecule 253.1, 208.2, 180.1, 301.1, and 349.2 were detected. Specific molecular
Fig. 7. Degradation pathway of Carbamazepine [284].
17
ions, mass fragment peaks, HPLC–MS library data, and the relevant these compounds should be considered a major threat to ecosystem.
chemical information were used to identify the products/intermediates. Several treatment methods have been adopted for the treatment of
Hydroxylation mechanism dominated during the transformation of hospital wastewater such as physical, biological, chemical, adsorption
carbamazepine into various byproducts by photodegradation process as and advanced oxidation are not efficient due to the complexity and
revealed in Fig. 5 (D and J) [284]. existence of pollutants as mixture in hospital wastewater, our findings
A preliminary degradation pathway of carbamazepine by BPO-180- shows that combination of advanced oxidation process with conven
72 was postulated based on the general laws of photocatalytic oxida tional method will be more suitable for successful degradation/removal
tion of organic molecules and the intermediates found by LC–MS of emerging contaminants in hospital wastewater. It is advisable not to
(Fig. 5). Photogenerated holes and hydroxyl radicals were the main treat hospital wastewater with sewer wastewaters since hospital
reactive species involved in carbamazepine degradation in aqueous wastewaters always have high concentration of pollutants. Therefore,
BiPO4 solutions [283]. The formation of HO• radicals in aqueous solu there is urgent need for every hospital to have mini treatment plants
tion was mostly due to the hole grabbing HO• of water or the reduction comprises combination of adsorption technology and advanced oxida
of O2 with electrons [284]. BiIII/BiV had a lower standard redox poten tion processes and other conventional methods to treat their liquid
tial (1.59 eV at pH 0) than HO⋅/HO for BiPO4 (1.99 eV). To begin with, wastes before release into the environment. Regulatory bodies are also
the produced HO• interacted immediately with carbamazepine to pro expected to involve in a continuous and periodic monitoring through
duce compounds A and E. (pathways I and III) [284]. The hydroxylation activation of strict enforcement and compliance to environmental safety
of aromatic rings by HO• radicals during the photocatalytic process has and sustainability.
been reported to be a key reaction in the sequential ring cleavage re
actions [284]. As a result, the HO• attacked the olefinic double bond on Credit author statement
the core heterocyclic ring, which was then oxidized by photogenerated
holes in a ring-rupturing process to yield product C (pathway II). The OJ, Ajala: Investigation, Writing-original draft. JO, Tijani:
intermediate A was further oxidized by the holes, yielding the Conceptualization, Data curation, Formal analysis, Investigation,
low-molecular-weight molecule B. Meanwhile, compound E was trans Methodology, Validation, Writing - original draft, Writing - review &
formed in two different ways in the reactions that followed. Product F editing. RB, Salau: Data curation, Formal analysis, Investigation. AS,
was generated by the attack of HO⋅ on the core heterocyclic ring’s Abdulkareem: Project administration, Resources, Supervision, Valida
olefinic double bond and an elimination process. It was subsequently tion, Visualization, Writing - review & editing. OS, Aremu: Data cura
subjected to hydrogen rearrangement process, yielding compound G. tion, Formal analysis, Investigation.
The intermediate G was further oxidized by incision to form compound
H. Product E was changed into compound I, which was comparable to
route II, in tandem with that process. Hydroxylation played a significant Declaration of competing interest
role in the transformation process. The intermediates C and I probably
oxidized to complex hydroxylated intermediates D and J in the presence The authors declare that they have no known competing financial
of HO• radicals, although no exact place for hydroxyl groups could be interests or personal relationships that could have appeared to influence
given from the fragmentation pattern. Finally, the ring-rupturing pro the work reported in this paper.
cesses oxidized the complex hydroxylated intermediates (D and J) and
low molecular molecules (B and H) to aliphatic compounds, which were References
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Results in Engineering 16 (2022) 100671

Contents lists available at ScienceDirect

A review of emerging micro-pollutants in hospital wastewater:

using characteristics such active component intake, water consumption

Table 1 To make matters even more complicated, concentrations of some

be under threat. The direct or indirect discharge of untreated hospital

Table 4 6.1. Physical techniques

Fig. 1. Different methods of treatment of hopsital wastewater.

intermediates D, E, implying that products B, C, and D, E may be

Fig. 3. The Degradation Pathway for Ciprofloxacin through photocatalysis [276].

Fig. 4. Degradation pathway of Norfloxacin through photocatalysis [279].

Fig. 5. Degradation pathway of Ofloxacin [281].

Fig. 6. Degradation pathway of Clofibric acid through photocatalysis [282].

Fig. 7. Degradation pathway of Carbamazepine [284].

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