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Treatment of spent metalworking fluids

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DOI: 10.1016/j.watres.2005.07.012 · Source: PubMed

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 ARTICLE IN PRESS

Water Research 39 (2005) 4051–4063

www.elsevier.com/locate/watres
Review
Treatment of spent metalworking fluids
Christina Chenga,, David Phippsa, Rafid M. Alkhaddarb
a
School of Biomolecular Sciences, Liverpool John Moores University, Byrom Street, Liverpool L3 3AF, UK
b
School of the Built Environment, Liverpool John Moores University, Clarence Street, Liverpool L3 5UG, UK
Received 17 August 2004; received in revised form 1 July 2005; accepted 8 July 2005
Available online 19 August 2005

Abstract

Metalworking fluids (MWFs) are widely used for cooling and lubricating during the machining process. The
worldwide annual usage is estimated to exceed 2
109 l and the waste could be more than ten times the usage, as the
MWFs have to be diluted prior to use. For UK industry the disposal cost is estimated to be up to £16 million per year.
Used MWFs cause high levels of contamination and rancid odours due to the presence of complex chemicals, biocides,
etc., so that their treatment and final disposal must be handled carefully. Conventionally this has been done by
combined physical and chemical methods but, with tightened legislation, these routes are no longer acceptable. Now,
biological treatment is being increasingly adopted as it seems to offer an alternative with the potential for significant
cost saving. However, there are significant difficulties in operating bioreactors, such as maintenance of the stability of
the microbial communities present in activated sludge plants (ASP). In order to resolve these problems, four major
areas need to be considered: (1) the composition of the spent MWF and its inherent biodegradability, (2) the
recalcitrant compounds existing in waste MWFs and their impact on microbes, (3) the nature of the microbial consortia
and means of optimising it, e.g, temperature and the practical design of the bioreactor and (4) the requirements for
nutrient supplements and optimal control conditions. The potential importance of understanding the microbial
community has been studied by the use of molecular biological techniques such as polymerase chain reaction (PCR),
denaturing gradient gel electrophoresis (DGGE), fatty acid methyl ester (FAME) and fluorescent in situ hybridization
(FISH). The application of attached biofilm bioreactors and thermophilic aerobic technology (TAT) has also been
studied. This review describes recent advances in each of these areas.
r 2005 Elsevier Ltd. All rights reserved.

Keywords: Metalworking fluids (MWFs); Biological; Wastewater; Treatment; Molecular techniques; Thermophilic

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4052
2. Development of treatment processes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4052
3. Biology of MWF . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4054
4. Pragmatic design and operational considerations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4058
5. Conclusions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4060

Corresponding author. Tel.: +44 151 231 2155.

E-mail address: [email protected] (C. Cheng).

0043-1354/$ - see front matter r 2005 Elsevier Ltd. All rights reserved.
doi:10.1016/j.watres.2005.07.012
 ARTICLE IN PRESS
4052 C. Cheng et al. / Water Research 39 (2005) 4051–4063

Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4060
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4060

1. Introduction tightening legislation relating to MWF disposal has

forced all industries to review their effluent treatment
Metalworking fluids (MWFs) have been used in processes or waste disposal options to meet the targets.
industry since ancient Egyptian times (BP, 1969), but In the USA, MWF users who generate 10–100 m3 are
their formulation and the study of their mechanism in required to treat their process discharge on site (Burke,
use has only been investigated during the last two 1991).
centuries. MWFs can be divided into two main types, oil Faced with all the tightening regulation, there have
based and water based. The oil-based MWFs can then been many discussions regarding used MWF treatment
be classified into two categories, namely straight oils and including chemical, physical and biological methods
soluble oils, and the water-based MWFs can also be (Sutton et al., 1985; Viraraghavan and Mathavan, 1990;
divided into two, synthetics and semi-synthetics (Wil- Kim et al., 1989, 1992a, b, 1994; Aki and Abraham,
bert, 1973; Foltz, 2002). The latter type of MWF is 1998; Portela et al., 2001; Ji et al., 2004). In the early
currently the main group used in engineering applica- 1990s, the dominant disposal methods were chemical
tions and has resulted in increased amounts of organic and physical processes; e.g., adding chemicals (lime,
chemicals being present in the MWF wastewater. In fact, alum, sodium aluminate, etc.) or polymers, and using
the complexity of the composition of waste MWF ultrafiltration and evaporation (Burke, 1991). Few
streams has created immense difficulties for the waste biological treatments were employed. Although MWF
disposal companies which deal with this type of waste, treatment plants have existed for a long time, many of
according to relevant reports and personal conversations them are not suitable to treat current spent MWFs
with several waste disposal providers (Sutton et al., because most of the treatment plants were designed to
1985; Sutton and Mishra, 1994; Spoors, 2003). There- deal with oil-based MWFs. (Sutton et al., 1985; Kim et
fore, this review paper attempts to compare many of the al., 1994). Modifications have been made to improve
methods used in spent MWF treatment and to provide these plants, so that they can be used for biological
an insight into the key areas for future research. treatment. Otherwise, plants using a type of hybrid
Before considering the details of treatment methodol- process involving combinations of biological and
ogy, a review of the latest legislation requirements is physical processes are also in use (DTI, 1998; Thomas,
essential in order to understand the standards to be met. 2001). Recently, genetic engineering has also been
First of all, the European Union demands that MWF employed to specify certain species that can enhance
manufacturers and suppliers provide products that are overall treatment performance (Van der Gast et al.,
both safe to use and ecologically acceptable during their 2004a).
production and use (BLF, 2003). Legislation regarding It seems that there are many treatment technologies
the regulation of MWFs relates not only to health and relating to the disposal of spent MWFs, but there is
safety but also to environmental concerns. In the UK, relatively little known about the effects of different
health and safety matters are monitored by the Health compositions on disposal methods, the need for supple-
and Safety Executive (HSE) and environmental issues ment requirements in treatment, the comparative
are policed by the Environment Agency (EA). Particular performance of different dominating microorganisms,
attention has been paid by the environmental authorities etc. Therefore, the purpose of this review is to: (1)
to used MWF disposal. The European Union Water summarise the compositions of MWFs listed in the
Directive (2000/60/EC) has also prioritised substances literature, (2) outline the variable microbial communities
and identified actions to be taken in order to minimise existing in both MWFs and in treatment systems, (3)
the impact on the environment. Furthermore, the describe possible safety, health and environmental
European Union Directive (2000/76/EC) has addressed impacts, (4) compare different types of reactors being
the problem of waste from incineration and provided an used in treating spent MWFs and (5) list relevant
even stricter framework aimed at reducing the negative advantages and disadvantages of each disposal method.
effect on the environment. The key pollutants to be
reduced are nitrogen oxides (NOx), sulphur dioxide
(SO2), hydrogen chloride (HCl) and heavy metals. 2. Development of treatment processes
(European Union, 2000a, b). Consequently it limits the
amount of spent MWFs being disposed off by means of MWFs are commonly used as coolants and lubricants
incineration. In other words, an alternative and cost in machining processes to increase productivity, prolong
effective option has to be identified and applied. The tool life, prevent corrosion, etc.; therefore there is a wide
 ARTICLE IN PRESS
C. Cheng et al. / Water Research 39 (2005) 4051–4063 4053

range of industrial users. A number of studies have been treatment, namely sand and granular activated carbon
carried out for treating the waste MWFs and these are (GAC), as they both provide not only surface area for
presented in Table 1. The majority of these studies were biological growth, but also adsorption capacity. The
carried out by Sutton et al. (1985), Sutton and Mishra latter was observed by Kim et al. (1989) but subsequent
(1994) and Kim et al. (1989, 1992a, b, 1994). Both treatment of the exhausted GAC was not discussed and
authors did their work in conjunction with the motor its toxicity could be significant. In addition, these studies
industry. The possible reason for this could be the by Kim et al. (1992a, b) appear to be the first to
massive amount of usage in the automotive industry, investigate whether aerobic or anaerobic conditions are
which ranges from 76 to 2839 m3/day (Sutton and better for waste MWF treatment. All their investigations
Mishra, 1994). Sutton et al. (1985), appear to be the were carried out with simulated wastewater consisting of
first to employ a fluidised bed reactor and demonstrate eight selected MWFs. Following their studies, they
its advantages. Fluidised bed operation is generally concluded that straight aerobic treatment could remove
believed to be capable of dealing with higher volumes of more than 88% COD, while only 64% could be removed
influent and providing a vast surface area for microbial anaerobically. The results indicated that the final
growth (Sutton et al., 1985; Fogler, 1999). Two types of effluent from an aerobic process gave a better perfor-
carrier have been used in the study of waste MWF mance. They also reported that there was up to 35% in

Table 1
MWF waste treatment research organisations and process employed

System Source of waste MWFs Influent COD COD removal References

(mg/l) (%)

Aerobic fluidised bed General Motors, 2101–2306 66–81 (Sutton et al., 1985)
process with sand as Sandusky, OH
carrier
Activated sludge John Deere Dubuque 560–1500 70–84 (Polak, 1986)
suspended-growth process Works, Iowa
Aerobic fluidised bed General Motors, N/A N/A (Hare et al., 1988)
process with sand as Sandusky, OH
carrier
Anaerobic fluidised bed Simulated waste MWFs 3300 60 (Kim et al., 1989)
process with GAC as
carrier
Packed bed reactor with Wascan Technical 145.9–715.2 64.1 (Viraraghavan and
peat as the packinga Institute, Canada Mathavan, 1990)
Anaerobic fluidised bed Simulated waste MWFs 1029–5324 68 (Kim et al., 1992b)
process with GAC as
carrier
Aerobic suspended growth Simulated waste MWFs 3200–3600 88 (Kim et al., 1992a)
Aerobic, anaerobic, and Simulated waste MWFs 1029–5324 72–100 (Kim et al., 1994)
aerobic/anaerobic with
fluidised bed reactor and
suspended growth
Aeration-suspended Cutting oil supplied by 560 26–78 (Deepak et al., 1994)
growth Indian Oil Co.
Integrated membrane Waste MWFs from 48000–68000 95–99 (DTI, 1998)
bioreactor system different industries
Aerobic fluidised bed Supplied by Olin Co. 3000 490 (Schreyer and Coughlin,
bioreactor with sand as Cheshire, CT 1999)
carrierb
Hydrothermal oxidation Supplied by Brugarolas, 1700–2882 38.7–97.4 (Portela et al., 2001)
Spain
Effluent from metal 48000 85 (Van der Gast et al.,
working processes 2004a)

GAC: granular activated carbon.

N/A: not available.
a
Specific for oil removal.
b
With pre-treatment.
 ARTICLE IN PRESS
4054 C. Cheng et al. / Water Research 39 (2005) 4051–4063

the system that was non-biodegradable when using an It also appears that MWFs can also be classified by
anaerobic process and a relatively lower percentage the additives present, which mainly consist of emulsi-
under aerobic condition. In fact, aerobic heterotrophs fiers, biocides, lubricating agents, pressure additives,
can certainly be expected to be the dominant micro- anti-foam agents, corrosion inhibitors and metal passi-
organisms because they are the major degraders for vators (Byers, 1994). Their individual properties can be
reducing the level of organic compounds in the waste used to measure MWF performance as well, e.g.,
stream. Although the aerobic process seems to be lubricating, cooling, corrosion inhibition and surface
superior to anaerobic operation in used MWF waste- finish functionalities (Greeley and Rajagopalan, 2004).
water treatment, the upflow anaerobic sludge bed The substances listed in Table 2 can also be briefly
(UASB) reactor was used to treat linear alkylbenzene classified by functionality. For example, chemicals used
sulfonate (LAS), a typical substance used in MWFs as a as lubricating additives would be from the oil category,
surfactant, under thermophilic conditions (Mogensen e.g., mineral oil, petroleum oil, etc., and in order to
and Ahring, 2002). eliminate mist forming, ester base oils or ester molecules
Van der Gast and colleagues have also carried out a have been used. Alkanolamines are widely known as
series of waste MWF treatment studies (Van der Gast corrosion inhibitors but other amines and fatty acids are
and Thompson, 2004; Van der Gast et al., 2001, 2002, also used. Some of the latest anti-corrosion additives
2003a, b, 2004a). In their work, the indigenous bacterial now have anti-wear properties too. In addition, boric
communities have been identified. Also comparisons of acid is also widely used in water-mix MWFs as an
the overall performance among activated sludge from additive for corrosion protection, pH buffering and hard
municipal sewage works, indigenous communities and water compatibility (BLF, 2003). Substances derived
bacterial consortia have been made. They proved that from alcohols or alcohols themselves are the main
introducing specific bacterial consortia was more effec- components in emulsifiers. Phosphate esters and sul-
tive. The technique of bacterial inoculation is named phurised esters are mainly used as pressure additives.
bioaugmentation, which is where additional organisms MWF bases are usually paraffins and chlorinated or
are added to enhance the treatment level when the sulphonated paraffins (Uniqema, 2003).
existing microorganisms are not degrading the pollutant MWFs play a major part in machining processes and
satisfactorily (Goldstein et al., 1985; Kaplan and Kitts, offer considerable benefits. However, the impact of
2003). using MWFs on safety, health and environment is also
The majority of the studies listed above attempt to significant, including harmful vapours in the workplace
identify the detailed composition of MWFs. However, environment either directly from the compounds or by
MWFs are proprietary products and manufacturers’ thermal degradation, toxic hazardous substances from
material safety data sheets (MSDS) normally give very synthetic MWFs and increased sludge production due to
little information for evaluating the impact of end-of- the difficulty of waste oil disposal. Other significant
pipe treatment. Waste MWFs can be straight machining health effects reported include occupational allergic
oils (non-emulsifiable), emulsifiable oil metalworking contact dermatitis directly linked to alkanolaminebo-
fluids, semi-synthetic metalworking fluids, synthetic rates (Sandin et al., 1990; Bruze et al., 1995), cancer risks
metalworking fluids, strong alkaline cleaners, mild associated with MWF exposure (Calvert et al., 1998), a
alkaline cleaners and mineral solvent emulsion cleaners correlation between pneumonitis hypersensitivity and
(Burke, 1991); but these names do not assist our Mycobacterium contamination (Moore et al., 2000) and
understanding of the precise compositions. An under- even stroke mortality has increased among workers
standing of the composition of MWFs is important for exposed to MWFs (Park, 2001). In addition to the
the design of waste MWF treatment routes, particularly toxicity of chemical substances, there are some patho-
in biological processes. Table 2 presents the known genic bacteria found in MWF samples, e.g., Pseudomo-
compositions of different types of MWF. From the nas aeruginosa and Klebsiella pneumoniae (Chazal,
composition, identification of the main sources of 1995). Despite these significant effects from waste
carbon, nitrogen, sulphate, hydrogen and phosphate MWFs and in-used MWFs, very few studies have
can be made and it can also help us decide the been carried out directly related to toxicity in the
requirement for supplements. In addition, knowledge environment.
of the type of biocide present in the system is essential
for a biological operation, as suppression of this activity
would be the first step in ensuring a positive environ- 3. Biology of MWF
ment for the microorganisms. There is a wide range of
biocides used in MWFs and typically they are metallic There are a variety of microbial communities existing
or chlorinated organic compounds designed for use as a in MWFs, leading to many interactions that influence
preservative, but other compounds are also used their quality or disposal treatment. Although significant
(Rossmoore, 1981). interest in the microorganisms existing in MWFs began
 ARTICLE IN PRESS
C. Cheng et al. / Water Research 39 (2005) 4051–4063 4055

Table 2
Summary of different metalworking fluid compositions

Type of MWFs Composition References

1. Synthetic Ethanolamines, Polyglycols, chlorinated or sulphonated (Baker et al., 1983)

paraffins, mineral oil
Polyglycols, glycol ether, alcohol amine salts, little or no (Sutton et al., 1985)
oil
Alkanolamine, emulsified oil (Polak, 1986)
Sodium O, O-diethyl dithiophosphate, (Sherburn and Large, 1999)
methyldiethanolamine (MDEA)
2-amino-2-ethyl-1, 3-propanediol (AEPD), 2- (2- (Geier et al., 2003)
aminoethoxy) ethanol
Ethanolamine; 2-aminoethanol, N,N0 - (Castrol, 2002a)
methylenebismorpholine
2. Semi-synthetic Triethanolamine (1800–2100 mg/l), sodium sulphonate (Schreyer and Coughlin, 1999)
(500–600 mg/l), 2-ethoxyethanol (80–100 mg/l)
Alcohol ethoxylate phosphate ester, polysulphides, di-tert- (Castrol, 2002b)
dodecyl, alcohol, C11-14-iso, C13-rich, sodium
sulphonate, 1-[2-(allyloxy)-2-(2,4-dichlorophenyl]-1H-
imidazole, N,N0 -methylenebismorpholine
3. Not stated whether Petroleum oil (1–5%), petroleum sulphonates(0.1–0.5%), (Foxall-VanAken et al., 1986)
synthetic/semi-synthetic linoleic acid (o0.1%),oleic acid
Fatty acids, alkanolamines, alcohols, polyglycols, amino (Kim et al., 1989; Kim et al., 1994)
acids, carboxylic acids, surfactants containing sulphur,
chloroalkanes, triazoles, triazines
Triethanolamine, cyclohexanamine, benzotriazole, indole,
heptanoic acid
Decanoic acid, hexadecanoic acid, 9-octadecenoic acid (Kim et al., 1994)
Mineral oil, sulphonated products, emulsifying agents (Deepak et al., 1994)
Alkanolamineborates, ethanolamines (Bruze et al., 1995)
Boric acid (BLF, 2003)
Mineral oil (89%), nonyl phenol 10 MEO (3.5%), fatty
acids (3.0%)
Nonyl phenol 4 MEO (2.7%), ethoxylated alcohols (1.8%) (Portela et al., 2001)
Benzotriazole (16%), amine propoxylate (54%), propylene (Van der Gast et al., 2003a, b)
(8%), formaldehyde-based biocide, benzotriazole,
dodecanedioic acid, lauric acid, sebacic acid, amine
propoxylate, glycerin, propylene glycol
4. Cleaners Silicic acid, dipotassium salt, ethanolamine; 2- (Castrol, 2003)
aminoethanol, alcohol, C8-10, ethers with polyethylene-
polypropylene, glycol monobenzyl ether, sodium
hydroxide, silicic acid, sodium salt, alcohol, C11-14-iso-,
C13-rich

in the mid-20th century, most of the investigations Traditionally, identification of bacterial isolates has
focused on MWF deterioration and epidemiologic been achieved by a cultivation approach but it is
studies for health and safety. Baker et al. (1983) were believed that less than 1% of the population present in
the first to examine bacterial communities existing in the environment is isolated and identified by means of
activated sludge systems for treating waste MWFs. culture-based techniques (Amann et al., 1995; Van der
Knowledge of biodiversity in the microbial mixtures Gast et al., 2001; WS Atkins Environment, 2000).
used for wastewater treatment is important in terms of Recent developments in biomolecular analytical techni-
determining their potential function in biodegradation. ques have enhanced the approach to understanding the
Methods used in identifying bacterial cells within the diversity of the microbial population in environmental
references cited in this paper are discussed below. samples. PCR–DGGE is a molecular approach to the
 ARTICLE IN PRESS
4056 C. Cheng et al. / Water Research 39 (2005) 4051–4063

analysis of the genetic diversity, and is based on the The techniques involve extracting DNA, PCR amplify-
separation of PCR-amplified 16S rDNA fragments by ing a sequence of DNA, and measuring the flourescence
polyacrylamide gels containing a linear gradient of intensity.
denaturant (7 M urea with 40% formamide at Researchers, who have attempted to isolate cultures
50–65 1C) (Lapara et al., 2000a, b; Van der Gast and from in-use MWFs or from waste MWF treatment, have
Thompson, 2004; Van der Gast et al., 2001, 2002, found Pseudomonas to be the main species with more
2003a, b). The molecular-based techniques involve ex- than seven species present. Among the seven, P.
tracting DNA from the environmental samples, PCR fluorescens, P. putida and P. stutzeri were frequently
amplification of a sequence of the DNA, and then isolated/detected from MWFs. Chazal (1995) also stated
DGGE separation of DNA fragments. The DGGE that the first two species are the major part of the
pattern obtained provides a rapid indication of biodi- indigenous microflora in MWFs. Several papers have
versity. By excising, re-amplifying, cloning and sequen- characterised the microorganism components with
cing specific DNA fragments, the components of the respect to the kind of bacteria present and the presence
microorganisms can be identified (Lapara et al., 2000a). of soluble protein in cell-free supernatants or in lipid
Fluorescence in situ hybridisation (FISH) is another extracts of pelleted cells from fluids. A summary of the
method to identify bacteria. The technique involves the bacterial groups observed in related MWF systems is
binding of complementary oligonucleotide probes (with presented in Table 3 and it appears that there are more
fluorescent label) to a target sequence in the host than 30 genera existing in either waste or in-use MWFs.
ssDNA. Gene probe is a single-stranded sequence of As these bacteria are present in both in-use and waste
DNA and can be designed specifically for the RNA of MWFs, they may well actually contribute to breaking
certain bacteria. Through hybridisation, the identifica- down organic compounds within bioreactors in spent
tion and quantification of desired cells can be achieved MWF treatment. As such, Baker et al. (1983) investi-
by epifluorescence microscopic detection. The advantage gated the bacterial distribution present in activated
of PCR–DGGE and FISH is that the methods are sludge reactors used for the degradation of MWFs. He
cultivation-independent, which means that the environ- reported that four bacteria, Acinetobacter, Alcaligenes,
mental microbial samples do not need to be cultured. Flavobacterium and Pseudomonas existed in the local
The techniques enable us to assess the extent of the plant, and these were also reported to exist in waste
microbial diversity without being limited to the cultur- MWFs. This proves that the indigenous MWF commu-
able microbes. nities could enhance the biodegradation of waste
Both phospholipid fatty acid (PLFA) analysis and MWFs, providing correct conditions to enrich these
fatty acid methyl ester (FAME) analysis are chemo- species were present. For example, another dominating
taxonomic techniques, based on analysis of bacterial genus in waste MWFs is Acinetobacter and species of
fatty acid originating from the cells, and provide a this genus are important as natural degraders of a
distinctive profile entirely unique to one strain (Lonon et variety of hydrocarbons in the soil (Foxall-VanAken et
al., 1999; Van der Gast et al., 2001, 2003a, b, 2004a). In al., 1986; Mattsby-Baltzer et al., 1989; Cloete and
other words, it allows the characterization and identi- Muyima, 1997). Presumably, species of Acinetobacter
fication of the bacteria in mixed cultures. The differ- could be used to form a bacterial consortium for
entiation between PLFA and FAME is that PLFA degrading wasted MWFs. A series of studies using
analysis only analyses phospholipid fatty acids originat- constructed bacterial consortia for the purpose of
ing from the cell membrane whilst FAME analysis degrading used MWF has been done by Van der Gast
covers all fatty acids present in the microbial cell. The and Thompson (2004), Van der Gast et al. (2001, 2002,
analytical procedures involve harvesting bacterial iso- 2003a, b, 2004a) According to Van der Gast et al.
lates, fatty acid extraction and gas/liquid chromatogra- (2004a), a bacterial consortium composed of Clavibacter
phy (GLC). The profiles generated from GLC are then michiganensis, Methylobacterium mesophilicum, Rhodo-
compared with the microbial identification database coccus erythropolis and P. putida has been successfully
(Microbial Identification System/MIS) to determine the applied to treat wasted MWFs and are 30–40% more
strains or their relatedness. The advantage of this effective than other biological treatments (Van der Gast
technique is that it is able to detect and identify bacteria et al., 2004a). Although the performance of the
and fungi although it is limited to the culturable constructed consortium was more effective as reported
microbes, as this technique requires microorganism by Van der Gast and Thompson (2004) and Van der
extraction prior to the analysis. Gast et al. (2004a), the potential difficulty of maintain-
Real-time PCR provides a more sensitive technique ing a stable bacterial consortium in a dynamic environ-
for direct cultivation-independent detection and quanti- ment needs to be addressed.
fication of environmental microbial samples by mon- Along with these microorganisms found in waste
itoring the fluorescence emitted during the reaction as an MWFs and in-used MWFs, there are a variety of
indicator of amplicon product (Khan and Yadav, 2004). microbes found in petroleum land treatment units and
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C. Cheng et al. / Water Research 39 (2005) 4051–4063 4057

Table 3
Partial list of bacteria isolated from in-use MWFs and spent MWFs

Organism Identification Location References

method

Mycobacterium immunogenum, Pseudomonas Genus-specific real- In-used MWFs (Khan and Yadav, 2004)
fluorescens time PCR assays
Alcaligenes xylosoxydans, Bacillus pumilius, B. PCR–DGGE, Wasted MWFs (Van der Gast et al., 2001,
sphaericus, B. marinus, B. oleronius, B. FAME 2002, 2003a, b, 2004a; Van
licheniformis, Brevibacterium brevis, der Gast and Thompson,
Brevibacterium lyticum, Brevundimonas diminuta, 2004)
Cellulomonas flavigena, Clavibacter michiganensis,
Comamonas acidovorans, Comamonas
testosteroni, Curtobacterium flaccumafaciens,
Gordona rubropertinctus, Methylobacterium
mesophilicum, M. radiotolerans, Nocardia
globerula, Enterococcus faecium, P. putida, P.
saccharophilia, Ralstonia pickettii, Rhodococcus
erythropolis, Stenotrophomonas maltophilia
Proteobacteria and, high G+C Gram + bacteria FISH Wasted MWFs/In- (Van der Gast et al., 2001,
use MWFs 2003a, b, 2004a)
Ochrobactrum anthropi, CDC Group B-1/B-3, Culture-based In-use MWFs (Lonon et al., 1999)
Alcaligenes faecalis ss faecalis, Tetragenococcus techniques, PLFA
halophilus, P. glathei, Streptococcus pneumoniae, analysis
Staphylococcus hominis, Corynebacterium
halophilus, Staphlococcus auricularis, P.
pseudoalcaligenes Comamonas terrigena,
Citrobacter freundii, Serpens flexibilis,
Xanthomonas oryzae, Micrococcus sp. P. dimuta,
Straphylococcus sp. Comamonas testosteroni, P.
fragi
Aeromonas, Pseufomonas, Flavobacterium, Culture-based Wasted MWFs (Sherburn and Large, 1999)
Bacillus techniques
Salmonella spp., Shigella spp., Vibrio spp., Gram Culture-based (Chazal, 1995)
(+) cocci, P. aeruginosa, P. putida, P. fluorescens, techniques
Klebsiella pneumoniae

P. pseudoalcaligens, P. stutzeri, Shewanella Culture-based In-used MWFs (Mattsby-Baltzer et al., 1989)

putrefaciens, Aerococcus viridans, Enterobacter techniques and GC
agglomerans, K. pneumoniae, K. oxytoca, Proteus analysis of 3-
vulgaris, E. coli, Citrobacter diversus, Citrobacter hydroxylauric acid
freundii, Serratia spp., A. viridans, Morganella for Pseudomonas
morganii, Corynebacterium spp., Streptococcus spp. determination
spp., fungi, yeast Candida spp., Mould Fusarium
spp.
Acinetobacter calcoacetucus subsp. Anitratus Culture-based Wasted MWFs (Foxall-VanAken et al., 1986)
subsp. Lwoffi, Acinetobacter haemolyticus, P. techniques
putida, P. stutzeri, P. alcaligenes, P. putrefaciens,
P. cepacia, Alcaligenes denitrificans
Acinetobacter, Aeromonas, Alcaligenes, Culture-based (Baker et al., 1983)
Caulobacter, Corynebacterium, Hyphomonas, techniques
Flavobacterium, Listeria, Microcyclus, Noraxella,
Pseudomonas, Seliberia, Sphaerotilus, Spirosoma
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4058 C. Cheng et al. / Water Research 39 (2005) 4051–4063

oil fields. Flavobacterium, Pseudomonas, Azoarcus 2, Abraham, 1998; DTI, 1998; Portela et al., 2001). Table 4
Azoarcus 1, Alcaligenes, Microbacterium, Bacteroides, a- provides a review of existing used MWF waste disposal
Proteobacteria, Rhodanobacter and Thermononas have methods. The capacity of each method listed was not
been found in petroleum land treatment units and stated in all studies. Brief estimates of evaporation,
Flavobacterium was found to be the most abundant ultrafiltration and chemical treatment were done by
when the degrading performance was at a relatively high Burke (1991) and were 25–3000, 50–15,000 and
level (Kaplan and Kitts, 2003). A thermophilic bacter- 50–1,000,000 gallons per day, respectively. For the
ium strain C2 was also found to be able to transform reverse osmosis system, capacity varies with design
crude oils to lighter hydrocarbons in an oil field located and can normally deal with 100,000 gallons per day
in East China (Hao et al., 2004). (Lin, 2004).
It can be seen in Table 4 that a further consideration
of the end products generated from the treatment
4. Pragmatic design and operational considerations process is required. For example, an air emission permit
will be needed for evaporation processes, and an
The treatment plants for waste MWF treatment have incineration procedure will be essential when the final
generally consisted of flow equalization, gravity separa- treatment is linked to membrane separation or a
tion of free oil, chemical emulsion breaking, floccula- filtration-related process. The design of the combination
tion, dissolved air flotation and clarification/filtration process listed in Table 4 combines a biological process,
for oil removal, when oil-based MWFs were the main an ultrafiltration system and a number of modules
type used (Sutton et al., 1985). However, oil removal has arranged in sequence. For example, a waste holding
become of relatively low importance in MWF disposal tank acted as a reservoir and an equilibration tank,
processes since synthetic and semi-synthetic MWFs have followed by a pre-filter to remove particulate matter.
gradually replaced oil-based MWFs. Organic matter The pre-filter is a coalescer separator allowing re-use of
removal is now the main task in MWF waste treatment. oily waste from the oil-rich effluent. There is a pre-
Although biological treatment is extensively considered treatment tank in which the waste was emulsified to aid
as being able to offer the most cost-effective option for biological treatment. Then the next stage was the
organic matter removal (DTI, 1998, 2000), there are aerobic biotreatment plant itself, and finally the ultra-
many different approaches to it (Burke, 1991; Aki and filtration unit for removing residual particles and oil

Table 4
Comparison of MWF waste disposal methods

Method References

Physical Treatment
Evaporation (Burke, 1991; MILACRON, 2000)
Membrane separation
Microfiltration (Burke, 1991)
Ultrafiltration (UF) (Burke, 1991; MILACRON, 2000)
Reverse osmosis (RO) (Burke, 1991; MILACRON, 2000; Lin, 2004)
Peat adsorption (Viraraghavan and Mathavan, 1990)
Chemical Treatment
Use of inorganic chemicals (Burke, 1991; MILACRON, 2000)
Use of cationic/anionic organic compounds (Burke, 1991; MILACRON, 2000; Yoshio and Masanori, 2001)
Hydrothermal oxidation (Aki and Abraham, 1998; Portela et al., 2001)

Biological Treatment
Aerobic activate sludge (Polak, 1986; Kim et al., 1992a, 1994; Deepak et al., 1994; van der
Gast et al., 2003a)
Anaerobic activate sludge (Kim et al., 1992b)
Aerobic sand fluidised bed reactor (FBR) (Sutton et al., 1985; Hare et al., 1988; Schreyer and Coughlin, 1999)
Anaerobic granular activated carbon (GAC) FBR (Kim et al., 1989, 1994)
Reed wetland (Ji et al., 2004)
Combination process
Activated sludge process plus ultrafiltration membrane (DTI, 1998)
technology
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C. Cheng et al. / Water Research 39 (2005) 4051–4063 4059

droplets (DTI, 1998, 2000; Thomas, 2001). Filtration Reactor temperatures in the studies mentioned in
technology has developed rapidly in the last 10 years and this paper ranged from 15 to 40 1C and according to
is employed in residential drinking water, as well as in Deepak et al. (1994), the COD was reduced as
industrial wastewater treatment. Generally, filtration temperature increased from 15 to 30 1C. Cheng
can be classified by the pore dimension, such as (Cheng et al., 2004) also increased temperature to
ultrafiltration, microfiltration, etc., and can also be 40 1C and found the COD removal rate was effectively
catalogued by the type of filtration materials, e.g., double that at 30 1C. This brings us to thermophilic
activated carbon, ceramic blocks, etc. (Lin, 2004). In technology, which emerged in the early 1950s (Lapara
waste MWF treatment, filtration processes are applied and Alleman, 1999). Several studies have been carried
as a pre-treatment or a post-treatment for biological out in thermophilic operation since, but there have not
degradation. When the filtration precedes the use of been many of these systems implemented at full
biological treatment, the function is mainly to eliminate scale, which may be due to the inconsistent results
the oil content. Alternatively, it is to retain the bio-solids (Couillard et al., 1989; Konopka et al., 1999; LaPara
in the system. Sludge, as a by-product, from the et al., 2000a, b, c, 2001b; Suvilampi et al., 2003). This
biological process will require further treatment, and is most likely because under thermophilic conditions,
either incineration or landfill could be the last stage. It many physico-chemical parameters, which are affected
should be borne in mind that there are many limitations by higher temperature, need to be taken into account
in disposing off sludge to landfill sites and therefore, either in the reactor design or operational conditions.
sludge elimination will be a vital issue in biological These physico-chemical parameters include viscosity,
processes. surface tension, gas–liquid solubility, diffusivity, and
With regard to biological wastewater treatment solid–liquid solubility. The first three parameters
processes, carbon, nitrogen, phosphorus and sulphur decrease with temperature and conversely, the last
are critical from the viewpoint of bacterial growth. two factors increase with temperature (Lapara and
From the composition of MWFs listed in Table 2, it can Alleman, 1999; Lapara et al., 2001a). Moreover, the
be seen clearly that there is sufficient carbon, nitrogen, narrower range of bacterial communities within the
sulphur, etc. Actually, in Kim’s research, the enrichment thermophilic category could reduce the consistency of
of ammonia in MWFs significantly interfered with the the bioreactor (Lapara et al., 2002).
COD analysis when chloride was present (Kim et al., Thermophilic aerobic treatment for waste MWFs
1994). As for phosphorous, it seems relatively absent can be still with potential, as it provides the possibility
and a supplement would improve the efficiency. of eliminating pathogenic bacteria. There is a high
According to Schreyer and Coughlin (1999), a phos- possibility of harbouring pathogens in waste MWFs
phorous supplement has improved the growth of because of its extent of microbial communities, and
microorganisms and the overall treatment performance. it has been proved that those pathogens can directly
Therefore, the level of phosphorous present in the harm human health. Although a UV disinfection pro-
treatment of spent MWF streams should be considered cess can be used for disinfection (Johnson and
either by adding it as a supplement or by combining Phillips, 2002), it could be more cost effective to use
other waste streams to enhance the overall efficiency. an all-in-one process, which includes both biodegrada-
Within the references cited in this paper, only Schreyer tion of pollutants and elimination of pathogens. There-
and Coughlin (1999) and Cheng et al. (2004) pointed out fore, a further investigation into the disposal of
that additional phosphate directly enhances the overall spent MWFs under thermophilic conditions may be
treatment efficiency. In Schreyer’s study (Schreyer worthwhile.
and Coughlin, 1999), the supplementation of phosphor- In addition to temperature, pH is also an important
ous was accomplished by replacing phosphoric acid factor that needs to be considered when operating a
with a portion of sulphuric acid in the breaking bioreactor. Among those studies discussed here, the pH
MWF emulsion stage, whilst in Cheng’s work (Cheng ranged from 6 to 8.5. As high pH helps biocide activity
et al., 2004), additional phosphate was added at the (Rossmoore, 1981; Sandin et al., 1990), alkaline
beginning of the treatment process according to the compound formations in the treatment process have
data generated from the industrial site where the to be limited. To our knowledge, the investigation
activated sludge was collected. On the industrial scale, carried out by Van der Gast and Thompson (2004)
the additional phosphate is added empirically on a is the only study relating to the effects of pH con-
daily basis. In terms of carbon source supplements, trol over waste MWF treatment and their results
Foxall-VanAken et al. (1986) also pointed out that showed that the optimal pH range for biological
with fatty acids as the sole carbon source, there is a treatment is between 6 and 7. It is important to note
more positive effect on strain growth than with the that in this study, a specific bacterial consortium was
naphthenic petroleum oil components as the sole reinoculated to the bioreactor for waste MWF treat-
carbon sources. ment. Therefore, whether the optimal pH range is
 ARTICLE IN PRESS
4060 C. Cheng et al. / Water Research 39 (2005) 4051–4063

the same with an undefined microbial mixture will need 5. Conclusions

to be considered.
Although investigations into either suspended growth Metalworking fluids (MWFs) have proved to be
or attached growth-activated sludge systems have been effective materials for improving machining processes,
taken into account in waste MWF treatment, attempts but in the concept of sustainability, care has to be taken
to directly compare the two operations to waste MWF in treating waste MWFs, as well as seeking an overall
treatment have not been made. Among these studies, improvement in their management, such as the use of
fluidised bed reactors were the only type of attached recycling procedures for increasing usage efficiency.
growth-activated sludge system used with sand and Technology for the latter would most likely be a
GAC as carriers (Table 1). The selection of carriers combination of reverse osmosis and solvent extraction.
directly affects the overall performance of wastewater For biological treatment, the predominant bacterial
treatment and recent developments in carriers have types found in used MWFs and in the used MWF
provided other alternatives, such as polypropylene beads biological treatment plants have been determined and
(Harris et al., 2001), polyurethane foam (Peng et al., their contribution to biodegradation in treatment
1997) and ceramic particles (Peng et al., 1999). Over all regimes has been shown to be significant. Issues needing
the biological treatments, the influent COD concentra- further investigation are:
tion varied from 1000 to 1,337,000 mg/l, which corre-
sponded to organic loadings from approximately 2400 1. determination of the effect of thermophilic condition
to 16,800 mg COD/day (Schreyer and Coughlin, 1999; control on MWF treatment efficiency for sludge and
Hilal et al., 2005). The treatment efficiency in terms of pathogenic bacteria elimination,
COD removal ranged form 60% to 99%. Most of the 2. determination of the effect of employing the biolo-
influent was simulated wastewater and most of the gical fluidised bed reactor (BFBR), using types of
studies were operated on a batch control basis. In other carrier on the overall treatment efficiency and on the
words, the hydraulic retention time (HRT) is equal to optimisation of operation conditions,
the sludge retention time (SRT). Whilst the operation 3. determination of the ratio of bioadsorption and
is continuous, HRT ranged from 3 h to 28 days in biodegradation in MWF biological treatment for
the reference cited in this paper. Another important further sludge disposal consideration and
factor for treatment facility design is food and micro- 4. determination of the effect of changes in influent
organism (F/M) ratio. The F/M ratio for conven- constituents on the bacterial community structure.
tional activated sludge systems ranges from 0.2 to
0.5 whilst for waste MWF treatment, it is from 0.63 to
0.22 (Polak, 1986), depending on the character of the Acknowledgements
waste streams. The source of activated sludge or
microorganisms employed for waste MWF in this review The authors thank the anonymous reviewers for their
paper included sludge originating from domestic and constructive criticism. Also, Dr. Glyn Hobbs and Ms.
industrial wastewater treatment plants and selective Ismini Nakouti (School of Biomolecular Science,
bacterial consortia. LJMU) for their valuable advice in molecular-based
Very little is known concerning the biodegradation techniques.
kinetics of MWFs. As mentioned above, Deepak et al.
(1994) seem to be the only ones who have evaluated the
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