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Super absorbent polymer replacement for disposable baby diapers

Technical Report · October 2019

DOI: 10.13140/RG.2.2.15095.98720

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 Super absorbent polymer replacement for disposable baby diapers
Nicolas Castrillon, Maria Echeverria, Heting Fu, Anurag Roy, Joseph Toombs
ME223 Commodity Polymer Project I • University of California, Berkeley • Fall 2019

Abstract
The diaper industry caters to a huge customer base comprising babies, the elderly as well as adults with certain medical conditions. Driven
by ease of use, a majority of diapers manufactured nowadays are of the disposable kind. Now, despite the overall convenience to
customers, one major drawback of these one-time use disposable diapers is that all of them invariably end up in landfills. It is noteworthy
to mention here that each of them has an estimated decomposition time of about half of a millennium owing to the presence of synthetic
components. A disposable diaper typically contains a number of polymers such as polyethylene, polypropylene, polyesters and
polyacrylates. Of these constituents, the most recent addition to the disposable diaper is the superabsorbent polymer (SAP) sodium
polyacrylate, which is non-biodegradable and which is the primary agent for water absorption and retention located in the core of the
commodity product. Having thoroughly reviewed the composition, manufacturing, functionalities, and environmental impact of disposable
diapers, the primary objective of this report is to propose a biodegradable substitute for sodium polyacrylate which could serve as a SAP. In
light of this, two materials that have shown promise are Poly(γ-glutamic) Acid (PGA) crosslinked by L-lysine and Gellan gum with
Jeffamine 130. The report also quantitatively asserts why the proposed material is better than the current one based on parameters such as
% biodegradability, water absorptivity, and retention time while discussing the associated development and challenges.

1. Introduction water per gram of cellulose fluff pulp, SAP can absorb up to
1000 g of water per gram of the polymer [3]. Sodium
The global industry of baby and adult diaper was valued at polyacrylate SAPs, are manufactured by mixing polyacrylic
US$65 Billion in 2018 [1], with the majority of the market acid (containing a carboxyl group) with a neutralizing agent
attributed to disposable diapers due to their convenience and such as sodium hydroxide in presence of a UV photo initiator
comfort. The average baby will consume about 4,000 and a crosslinker. Once in solution stage, the hydrogen in the
disposable (single-use) diapers in his/her lifetime [2], making carboxyl group detaches and sodium ions replace it instead,
these consumer products one of the most prevalent in landfills. thereby neutralizing the negatively charged carboxyl in the
The basic construction of disposable diapers consists of an process. This is generally followed by irradiation with intense
absorbent pad, or “core,” sandwiched between two layers of UV light, thus creating sodium polyacrylate. Under the
non-woven fabric that guide moisture towards the hydrophilic influence of multi-functional cross-linking agents, it is
core of the diaper while keeping the skin of the baby ultimately converted into a gel through radical addition
comfortable. Once the moisture reaches the core it comes in polymerization. The gel is thereafter dried, crumbled, and
contact with a sodium polyacrylate powder, a semi-crystalline ground into a fine powder using ball milling and finally
superabsorbent polymer (SAP). As their name suggests, SAPs screened out to obtain specific particle sizes. The SAP powder
are characterized by their unique and remarkable ability to is commonly used in dry granular powder form as described in
absorb 100 - 1000 times their mass in deionized water [3]. the following sections.
Also, disposable diapers have comfort features, including an The diaper’s absorbent pad is a matrix made up of two
elastic band to prevent leakages and adhesive tape to keep the essential parts. Manufacturers have optimized the two
diaper in place at the hips. constituents to suit the purpose of maximum water retention.
The earliest disposable diapers were made with primarily The two constituents are as follows:
biodegradable components, a thick layer of absorbent cellulose a) A fine (hydrophilic) polymer powder i.e. sodium
and thin synthetic comfort layer. With the advent of SAPs, polyacrylate which behaves like a tiny sponge exhibiting large
modern diapers are typically composed of 43% fluff pulp, 27% water retention capacity. At the microscopic level, the polymer
SAP material, and 30% of other materials making up the non- molecules are long (rope-like) chains with many functional
woven sheets [4]. These components give the diaper a thin and side groups, some of which interact with the water molecules
flexible overall construction at the cost of reduced while others chemically cross-link with other polymer
biodegradability due to the high percentage of non- molecules. This cross-linking process aids in ensuring a gel
biodegradable SAP. In this report, we investigate alternative network formation that absorbs enormous quantities of water
absorbent polymers that could reduce the environmental instead of dissolving in it.
impact of diapers by enhancing the biodegradability of the b) A fibrous material, for example, wood pulp. These
synthetic components in diapers. We introduce several fibers play the role of tiny straws which draw water from the
performance metrics to quantitatively compare the potential inner portion of the diaper and distribute it throughout the
alternatives: liquid absorbance or swelling, moisture retention absorbent layer matrix, essentially avoiding a phenomenon
time, and degree of biodegradability. called gel blocking. Gel blocking occurs when the outermost
layer of the pad absorbs water very rapidly, forming a gel
2. Manufacturing of Diapers which prevents further water content from permeating the bulk
of the intermediate absorbent layer, severely debilitating the
Formerly made from only cellulose fluff pulp, modern- overall functioning of the diaper.
day diaper manufacturers prefer to add SAP powder in the Looking into the construction, the absorbent pad is
absorbent layers which are clean, dry and granular in texture. sandwiched between two sheets of nonwoven fabric, which
This powder, upon exposure to water, forms a slurry and provide a steady shape, conformity and prevent leakage from
gradually absorbs the water transforming into a soft rubbery the sides. The top sheet (polypropylene) is permeable so as to
gel. When compared to the absorptivity of dry fiber, 12g of absorb and transmit the body fluids to the adjacent absorbent

1
pad, while the bottom sheet (polyethylene) is impermeable to give strength to prevent gel blocking and reducing the number
ensure leakage prevention from the other side of the diaper. or strength of crosslinks that must be broken in the
The pad’s layered construction is conducive to a roll-based biodegradation process.
conveyor belt assembly that occurs inside a long forming
chamber. The chamber has various pressurized nozzles at the Biodegradability
top through which either fibrous material or polymer powder In this report, the level of biodegradability of a
can be dispersed onto the underlying conveyor belt. A vacuum polymer is compared using biochemical oxygen demand
underneath the belt flattens the sprayed fibers. It is only after (BOD) analysis. In a basic test, the BOD percentage is the
the bottom fibrous layer of the pad is formed that the nozzles difference in the amount of microbial oxygen consumption
begin spraying a mixture of fibers and SAP powder. The final between a control sample and the subject sample which
layer, also primarily composed of fibers, is levelled by a roller contains the polymer to be degraded, as in Eq. 2 below.
which also removes excess fiber and ensures necessary
thickness uniformity. As a result of this multi-layered 𝐵𝑂𝐷
deposition, the SAP component is positioned centrally between 𝑚0 20345#67803 9: 459;<27 − 𝑚01 20345#67803 9: 2037>0?
the fibrous layers preventing the possibility of gel blocking. = 1
𝑚60?:#<> 45947@32<
Once the three components (absorbent pad, top and (2)
bottom sheets of nonwoven fabric) have been formed
individually, they are assembled together by passing the
The percentage biodegradability or biodegradation is
absorbent pad through a conveyor belt with the pre-applied determined by correcting the BOD for the theoretical oxygen
bottom sheet. The top sheet is placed onto the stack and the
uptake (ThOD) of the medium calculated by theoretical
assembly is connected together by a series of gluing, heating
models. The percentage biodegradability is expressed as in Eq.
and ultrasonic merging steps. The completed long layered rolls
3 [6].
are lastly cut into single unit disposable diapers, packed, and
shipped. MNO
%𝐵𝑖𝑜𝑑𝑒𝑔𝑟𝑎𝑑𝑎𝑏𝑖𝑙𝑖𝑡𝑦 = PQNO (3)

3. Chemistries and mechanisms of key metrics Glass transition temperature

Liquid Absorbance/Swelling When the polymeric powder (sodium polyacrylate)
Sodium polyacrylate and the proposed alternatives in comes in contact with water, a chemical rearrangement of
the following sections each have carboxyl side groups. The atoms transpires which causes water molecules to ‘stick’ to the
carbonyl and hydroxide groups of the carboxyl group being ions (sodium and carboxyl) in the solution. This leads to the
electron donors and acceptors, respectively, give the SAP a formation of a gel that expands in volume to a great extent. For
propensity to form hydrogen bonds with polar water molecules this volumetric expansion to occur, it is important that the
when hydrated. During hydration, two primary reactions occur: chains of the polymer be flexible enough to slide past one
(i) the sodium dissociates from the polymer chains and attracts another at the ambient temperature. Accordingly, the glass
polar water molecules while free to move about in the gel; (ii) transition temperature (Tg) of the swollen SAP should be lower
the now deprotonated carboxyl groups exhibit repulsion with than the room temperature such that the chains have the
each other while forming hydrogen bonds with free water required mobility. The Tg should be low enough that the
molecules. Both of these reactions contribute to the total polymer exists in the ductile regime ensuring conformity and
swelling of the polymer: (i) the sodium ions, while free to snug contact with the user, accommodating motions (walking,
move locally, are trapped within the gel because of weak sitting, sleeping, and crawling) without releasing the fluid
attraction to the carboxylate anions, therefore the osmotic already absorbed.
pressure increases; (ii) the repulsion of the carboxylate anions
additionally expands the polymer network by electrostatic 4. Environmental Impact
pressure. The swelling and absorption of water stops when the After the introduction of SAP the usage of diapers
sum of these pressures equals the bonding strength of the increased over 44% [7] and absorbent hygiene products such
crosslinked network. Naturally, the degree of crosslinking of as diapers, feminine care and incontinence products currently
the polymer has a significant effect on the degree of swelling, account for a 1.5-6.3% of the municipal solid waste in Europe.
polymers that are highly crosslinked do not have as much However, the SAP inception also brought a substantial
freedom to expand and thus exhibit weak absorption [5]. The reduction on the weight of the diaper of about 50% from 65g in
degree of swelling is a quantifiable indication of the polymer’s 1987 to 33g in 2013 [8]. The impact of the weight reduction
ability to absorb liquid and we define the degree of swelling as and the innovation in materials that make up the diaper has
in Eq. 1. been measured with a life cycle assessment (LCA) technique
#$%& '#()*
𝑆= (1) [4]. The analysis found a reduction of the fossil-based CO2 by
#()*
14% explained by a significant reduction in the amount of pulp
Where mwet is the mass of the hydrogel after absorbing a
liquid and mdry is the dry as manufactured mass. Finally, the used, reduction of 30% in NOx and a 15% decrease in SOX
light crosslinking of the polymer allows for a large degree of with respect to 1987 data. In terms of emissions into water, the
swelling but prevents complete dissolution in aqueous media. report showed a reduction of 70% in chemical oxygen demand
While complete dissolution is undesirable in the diaper, (COD) and absorbed halogenated organic compounds (AOX);
biodegradability is of concern for our proposed alternative. being improvements on bleaching process and reduction of
Therefore, there exists a tradeoff between optimizing the level pulp content/replacement with SAP the main reasons for the
of crosslinking needed to prevent dissolution of the SAP and reduction. On the other hand, sulphates and other inorganic

2
compounds increased by 23% for the same reason. Overall,
there has been a reduction in water usage and air emissions due
to the introduction of SAP since 1987, improving not only the
performance of the diaper but the environmental impact on
most of the indicators measured [4]. The fact is that innovation
in materials, recycling, biodegradability and packaging is key Figure 3. Predicted structure of gellan gum-Jeffamine hydrogel
to further reducing environmental impact. after crosslinking, represented by gellan gum (blue), Jeffamine
Recyclability of diapers is possible but its cost and lack of (red), and zero-length EDC/NHS crosslinking points (yellow) [9].
market for reuse of the product makes it almost prohibitive.
Although progress has been made to recycle and upcycle The study found that liquid absorbance of the
soiled diapers if we can create materials that can degrade in hydrogel was affected both by the acyl forms of gellan gum
bacteria-rich soil we create a solution for processing waste and employed and the quantities of EDC/NHS crosslinker. Test
preventing landfill waste accumulation and incineration. samples with the highest liquid absorbance were prepared with
high-acyl gellan gum (GGHA) and lower quantities of
5. Proposed materials EDC/NHS. In other words, these test samples have less
crosslinking, which results in adequate water absorbance of
Option 1: Gellan gum and Jeffamine 130 + EDC/NHS 145 g/g. Furthermore, the samples demonstrated excellent
An international collaboration at the University of water-retention ability, capable of a 450-minute water retention
Michigan provided an alternative hydrogel for sodium period. Also, its inherent properties make this replacement
polyacrylate [9]. Researchers obtained a biodegradable SAP by hydrogel suitable for arid climate or long-term storage before
crosslinking gellan gum and Jeffamine 130 (O,O’ -bis(2- use. The authors claim that the polymer is biodegradable after
aminopropyl)-polyethylene glycol) with [1-ethyl-3-(3- its intended use of controlled water or chemical release in
dimethylaminopropyl) carbodiimide hydrochloride] (EDC) and agricultural applications but do not provide experimental
N-hydroxysuccinamide (NHS). Gellan gum can be obtained in evidence to support the claim. In a separate study, the
a high acyl or low acyl form, as shown in Figure 1. When biodegradability of gellan gum was shown to be highly
hydrated, high acyl gellan gum, its natural form, forms a soft dependent on the acyl percentage. High acyl percentages have
elastic hydrogel while the deacylated low acyl gum forms a a greater number of large acyl side groups which can partially
stiffer more robust hydrogel. The chemical structure of the inhibit the gelling process resulting in a weaker gel that can be
primary crosslinker Jeffamine is shown in Figure 2. EDC/NHS degraded more rapidly, when compared with the stiffer low
acts as a zero-length secondary crosslinker which joins the acyl form [10]. Another study showed a biodegradability
amine groups of Jeffamine with the carboxyl groups of the dependence on the EDC/NHS content of a collagen-based
gellan gum forming an amine bond. The predicted structure of material. Low EDC/NHS crosslinker concentration degraded at
gellan gum-Jeffamine is shown in Figure 3 [9]. The advantage a faster rate than high concentration. These studies suggest that
of EDC/NHS combination is that urea is the only by-product of the high absorptivity gellan gum-Jeffamine polymer may be
the reaction, and it is water soluble and non-toxic. Thus, the biodegradable if high acyl gellan gum is used and the
manufacturing process of the hydrogel produces minimal EDC/NHS content is carefully chosen to balance the stiffness
cytotoxic waste which is an important consideration when and absorptivity of the polymer with the biodegradability.
choosing an alternative to sodium polyacrylate [10].
Option 2: Poly(γ-glutamic) Acid
Perhaps a more promising alternative is a poly(γ-
glutamic) acid (PGA) based hydrogel synthetized from a
microbial source. The polymer structure of PGA is shown in
Figure 4. PGA is a ubiquitous amino acid used in the synthesis
of proteins, which facilitates in the industrial production using
a mutant Brevibacterium flavum, yielding roughly 40 g/L in 2
days [11]. Naturally, PGA occurs in organisms by the
condensation of glutamate and ammonia, as shown in Figure 5,
an essential role in the metabolism of nitrogen. In humans,
PGA facilitates natural processes in the intestines, regulates
acid-base balance in the kidneys, activates immune cells, and
feeds cancerous cells. Studies such as [12] by Kunioka show
that PGA hydrogels are efficient agents for the purification of
turbid water.
PGA is water-soluble and biodegradable linear
Figure 1. Chemical structure of high acyl and low acyl gellan molecule with a high molecular weight between 100,000 to
gum. 1,000,000 g/mol. The synthesis of cross linking PGA was
published in 2011 by Murakami et al., a collaboration between
Japanese researchers at the Kagawa Industrial Technology
Center and Keio University [13]. Murakami et al. noted that
the crosslinking agents that are commercially available are
derivatives of petroleum, substances that do not lend
Figure 2. Chemical structure of Jeffamine. themselves to “green” chemistry. Additionally, PGA is

3
typically self-crosslinked by special γ-irradiation equipment. A at 25°C and the findings are summarized in Table 1Similar to
green solution that forgoes γ-irradiation is crosslinking by L- the gellan gum-Jeffamine hydrogel, we note that the
lysine, a bio-based amino acid for arresting the spread of absorbance and biodegradability of the PGA with L-lysine gel
herpes. depends heavily on the degree of crosslinking, so optimization
of the polymer’s components would be necessary before
application in the diaper industry

6. Discussion regarding product development

Since these products are in contact with human body

fluids and waste, switching to a new material will require
technical assessments to evaluate risk for systemic toxicity
(including toxicity due to ingestion) and local effects (skin
irritation, sensitization, contact dermatitis) [14]. For example,
one of the major toxicity-related issues seen with products
based on super absorbent polymers is a condition called toxic
shock syndrome (TSS). This syndrome is caused when the
normal bacteria (found on the skin, nose, armpit, groin or
Figure 4. Molecular structure of the PGA gel, composed of vagina), i.e. Staphylococcus aureus, over grows and produces a
poly(γ-glutamic) acid (PGA) in blue crosslinked by L-lysine in red toxin that then enters the bloodstream affecting some
[13]. individuals [15]. To examine this effect, it would be
advantageous to measure bacteria growth (colonization) in the
new SAP media at different times and compare it to the
The Murakawi study found that crosslinking the PGA
sodium polyacrylate SAP. If there is an increase in bacteria
with L-lysine showed high water absorption above the range of
colonization, antimicrobial agents such as zinc oxide [16]
the current material, sodium polyacrylate, and within the same
could be added either to the SAP absorbent layer or the liner of
range as pure PGA crosslinked by γ-irradiation. The full
the diaper to reduce the risk of bacterial overgrowth.
findings are shown in Figure 6 and these behaviors are
Another factor that should be evaluated is a potential risk
summarized in Table 1.
of acute ingestion and direct contact with the skin. It has been
PGA crosslinked by L-lysine shows improved
demonstrated that accidental ingestion of SAP found in the
biodegradability compared to the current SAP, sodium
core of the diapers (small granules) does not lead to an
polyacrylate. According to Kunioka, PGA is water soluble,
increased health risk for babies (no choking or suffocation);
hydrodegradable, and biodegradable hydrogel, and the degree
the inertness of the polymer prevents an internal toxic response
of degradation depends on the density of crosslinking by the L-
[14]. The SAP is not expected to contact the skin as it is
lysine; a higher degree of crosslinking yields a lower extent of
enclosed within the fibrous core matrix between many layers
degradation for the same amount of time and temperature since
of polymer sheeting that prevent leakage. Direct skin contact
more chain scission events at the amide group must
and ingestion, while unlikely, are not expected to induce any
occur.Figure 7 shows the biodegradability of PGA with L-
lysine as measured by Murakami with activated sewage sludge negative reactions from the user.

Figure 5. Synthesis of glutamine by the condensation of glutamate and ammonia.

Table 1. Comparison of properties between the current polymer (Sodium polyacrylate) and two “green” alternatives (Gellan gum with
Jeffamine, PGA with L-lysine).

Material Water Absorptivity (g/g) %Biodegradability (BOD Moisture Retention Time

method)

Sodium polyacrylate 100 - 1000 Not Applicable 96 h

(30C, 1atm) [17]

Gellan gum with Jeffamine 77 - 145 Not Available 7.5h

(deionized water, 70C, 1atm)

PGA with L-lysine 900 - 2,750 60% in 20h Not Available

4
 7. Conclusion

In this report we propose two alternatives to the current

state of the art SAP, sodium polyacrylate. Each polymer has
hydrophilic electronegative carboxyl side groups which
retain polar water molecules and swell when hydrated. First,
a polysaccharide derived gellan gum-Jeffamine polymer
shows water absorptivity and retention time on the same
order of magnitude as sodium polyacrylate but the degree of
biodegradability is unclear. The individual components of
the polymer may be degradable as shown by independent
. studies but the researchers describing the chemistry of the
Figure 6. Water absorption by mass (g/g) of PGA for varying L- polymer do not provide experimental results required to
lysine crosslink densities (y-axis on right, with ⃞ markers) [13]. reach a conclusion about the biodegradability. The second
alternative, an amino acid-based polyglutamic acid-L-lysine
crosslinked polymer, shows more encouraging results. PGA
water absorbance is about twice that of the state of the art
and it shows exemplary degree of biodegradability in a
microbial BOD analysis. However, water retention may
present a challenge for this chemistry. Nevertheless, for
either alternative, the degree of crosslinking must be
carefully adjusted to achieve the optimum balance between
stiffness and related resistance to dissolution in water and the
biodegradability of the polymer. High degree of crosslinking
results in a stiffer polymer which is able to resist the gel
blocking phenomenon as well as dissolution before gel
formation but it also limits swelling and consequently water
. absorptivity. Low degree of crosslinking allows the polymer
Figure 7. Extent of biodegradability over time of PGA to expand and absorb up to 2,750 times its weight in water,
crosslinked with L-lysine (solid line), as measured by the BOD in the case of the PGA SAP. Of equal importance, is the
method [13]. improved ability of lightly crosslinked hydrogels to
biodegrade at a faster rate. Because the PGA is amino acid-
In terms of product development the main challenge is based, toxicity is unlikely to be a major concern. Finally, we
making the material at industrial scale, not only to keep the suggest a lightly crosslinked PGA has the best potential to
cost down but to fully replace fuel-based SAP currently used. replace the current sodium polyacrylate SAP because of its
The environmental impacts of the new type of SAP additive superior water absorbance and ability to significantly reduce
would have to be assessed following the life cycle the accumulation of diapers in landfills because of its degree
assessment methodology (International Organization for of biodegradability in microbial BOD testing.
Standardization, 2006a, 2006b). Additionally, following
EDANA protocols, the performance of the new product
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