Surfaces and Interfaces 27 (2021) 101532

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Surfaces and Interfaces

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Removal of surfactants in greywater using low-cost natural adsorbents:

A review
Shreya a, Akshaya Kumar Verma b, *, Aditya Kishore Dash c, Puspendu Bhunia d,
Rajesh Roshan Dash d
a
Environmental Science and Technology, Faculty of Engineering and Technology (ITER), Siksha ‘O’ Anusandhan (Deemed to be University), Bhubaneswar, Odisha 751
030, India
b
Department of Civil Engineering, Faculty of Engineering and Technology (ITER), Siksha ‘O’ Anusandhan (Deemed to be University), Bhubaneswar, Odisha 751 030,
India
c
Bio-fuel & Bio-processing Research Center, Faculty of Engineering and Technology (ITER), Siksha ‘O’ Anusandhan (Deemed to be University), Bhubaneswar, Odisha
751 030, India
d
School of Infrastructure, Indian Institute of Technology Bhubaneswar, Odisha 752 050, India

A R T I C L E I N F O A B S T R A C T

Keywords: Water scarcity problem due to both natural and human-made phenomenon is on the rise. Development and
Greywater implementation of efficient and cost-effective methods to treat and reuse wastewater has become a subject of
Surfactants prime importance. Greywater constitutes approximately 70% of total wastewater from a household, if treated
Adsorption
can address major water shortage problems. The current review is focused on the use of low cost materials as
Low-cost natural adsorbents
adsorbents for the removal of surfactants from gray water. Based on the literature survey, common adsorbents
like wood and activated carbon have long been used as conventional adsorbents to remove typical greywater
pollutants. In particular, waste materials as low-cost adsorbents tested in the past for the removal of surfactants,
which constitute major proportion of pollutants in greywater, have been the focal point of the present study. The
values of typical parameters of wastewater as studied by various researchers were closely observed and were
found as pH 6.2–9.4, turbidity 20–444 NTU, total dissolved solids (TDS) 237–2385 mg/L, chemical oxygen
demand (COD) 58–1340 mg/L, biochemical oxygen demand (BOD5) 42.1–6250 mg/L, TSS 25–1852 mg/L and
surfactants 3–118 mg/L. Myriads of research have investigated the potential use of agricultural waste as cheap
and natural adsorbents for the removal of pollutants from both industrial and domestic wastewater. The fact that
some of such bio-sorbents have been tested specifically for removing surfactants from greywater makes it an
untouched and naive field of research. Adsorbents that have been tested include granite sand, granular charcoal,
dolochar, rice husk, coconut shell, zeolites etc. Such studies have not only portrayed a wide range of removal
efficiencies but also depicted a pH dependent adsorption process. In a nutshell, there is a tremendous scope to
explore such cost-efficient and simple alternatives and subsequently be implemented in the near future.

Development Program (UNDP) goals, by 2030, it is aimed to reduce

1. Introduction
In today’s era, fresh water sources are rapidly on the decline. Un­
restricted anthropogenic activities have led to increasing problems of
water pollution, stress and related diseases. Many regulatory authorities
and international agencies have given importance to the reuse and
recycling of wastewater. Therefore, the need for treatment of waste­
water generated from industries and households has become an
important focus of current research. As per the United Nations
water pollution, improve the water quality, reduce discharge of toxic
substances into the environment and focus on recycle and reuse [1].
Recent reports furnished by the United Nations reiterate the problem of
water stress faced by 700 million people in 43 countries. It is approxi­
mated that 663 million people do not have access to uncontaminated
and reliable source of drinking water. In addition, roughly 1.8 billion
people are without good quality water considered to be safe for human
consumption [2].
A typical household generates two types of wastewater viz.:

* Corresponding author.
E-mail addresses: akshayakumarverma@soa.ac.in (A.K. Verma), adityadash@soa.ac.in (A.K. Dash), pbhunia@iitbbs.ac.in (P. Bhunia), rrdash@iitbbs.ac.in
(R.R. Dash).

https://doi.org/10.1016/j.surfin.2021.101532
Received 17 June 2020; Received in revised form 7 September 2021; Accepted 9 October 2021
Available online 13 October 2021
2468-0230/© 2021 Elsevier B.V. All rights reserved.
Shreya et al. Surfaces and Interfaces 27 (2021) 101532

Nomenclature SBR sequencing batch reactor

UASB upflow anaerobic sludge blanket reactor
BOD bio-chemical oxygen demand SDS sodium dodecyl sulfonate
TN total nitrogen CPC cetylpyridinium chloride
TP total phosphorous DTAB dodecyltrimethylammonium bromide
TSS total suspended solids HTAB hexadecyltrimethylammonium bromide
FC fecal coliform SDBS sodium dodecyl benzene sulfonate
TC total coliform PZC point of zero charge
Lpcd liters per capita per day DPC dodecylpyridinium chloride
TDS total dissolved solids DPCl dodecylpyridiniumchloride
COD chemical oxygen demand BCl benzethonium chloride
XOCs xenobiotic organic compounds BCl sodium dihexyl sulfosuccinate
NTU nephelometric turbidity unit CAS chrome Azurol S
MPN most probable number CMC critical micelle concentration
LAS linear alkylbenzene sulfonate

greywater and black water. Wastewater stream coming from bathroom/
showers, kitchen sinks/dishwashers, hand basins, washing machines
etc. excluding the one coming from toilet flushing is termed as grey­
water. It constitutes 50–80% of the total household wastewater gener­
ated [3–5]. As the black water effluent which consists of urine, feces and
toilet paper does not enter the greywater stream, the latter is considered
as less polluted. This gives us an opportunity to recycle and reuse
greywater that would greatly reduce the demand for first use water and
help to conserve our depleting water resources. Greywater treatment at
decentralized stations (i.e. household or community level) will not only
help in reducing load on the wastewater treatment plants but also sub­
sequently pose lesser stress on infrastructures located downstream for
catering to water demands by various sectors [5,6]. On the other hand,
mixing the two streams reduces future prospects of reusing compara­
tively clean wastewater after requisite purification steps thereby
providing alternative water sources closer to the points of use. This in­
dicates shorter length of pipes and less pumping as about 80 to 90% of
the capital is spent on collection and pumping. Such infrastructural
energy requirements and cost can be cut down drastically if decentral­
ized wastewater systems are adopted. Hence source separation plays a
pivotal role in overall reduction in energy demand [7,8].
Myriads of conventional protocols like chemical/electro-coagulation
[9], ion exchange, electrolysis, photo-catalytic degradation [10,11] and
biological treatments exist for removal of heavy metals [12–14], dyes
[15,16] and other toxic components present in wastewater. Usually,
adsorption is considered to be one of the best and simple techniques for
the removal of toxic and noxious impurities from wastewater in com­
parison to the aforementioned techniques. Lower waste, higher effi­
ciency and simple and mild operational conditions are some of the
important advantages of adsorption process [17–22]. Low-cost adsor­
bents are typically discarded/waste products from a process
(manufacturing etc.), agricultural waste, food organic waste and other
microbial biomass that have a potential to be utilized as an adsorbent
[23]. Such cheap and affordable products can be put to a better use after
their partial modification aiming to improve the adsorption capacity in
purifying wastewater rather than being thrown away in the environment
[24]. Therefore, the focal point of this study is to present a compre­
hensive review on the possible use of low cost waste materials in their
original and/or modified forms for the removal of surfactants from gray
water which can be reused further for any secondary purpose.
2. Greywater recycling in India
The Ministry of Drinking Water and Sanitation, The Government of
India has released a book on Greywater management in rural India
(https://sujalswachhsangraha.gov.in/sites/default/files/gray_wate
r_Management_Resource_Book_GoI.pdf). As the population of India may
reach close to 1.65 billion by 2030, the management of greywater in
rural India will need innovative solutions to address the challenge. Many
feasible treatment options both on site and off site exist including small
bore drainage systems that are cheaper and less invasive. Household
level greywater management may include soak pits, leach pit, magic pit
and kitchen garden. Village level greywater management may include
waste stabilization ponds, constructed wetland, phytorid technology,
anaerobic baffled reactor, waste stabilization ponds etc. The goal has
been to develop greywater management systems at all three levels viz:
household-level, community-level, and the village-level. A review by
Sushmitha et al. [25] refers to greywater treatment options and reuse in
India. It is inferred that though a combination of RBC and physi­
ochemical process has shown efficient removal of pollutants, huge space
and high investment is an issue in India. Therefore, constructed wet­
lands such as reed bed treatment would be an economical option. The
issues of wastewater reuse in India arise from lack treatment and so
simple, low-cost, low- maintenance, low-skill and user-friendly methods
must be adopted. In India, wastewater coming from bathroom and
kitchen has been utilized to grow coconuts, banana, colocassia, etc. for
many centuries. Now, the concept to reuse the greywater is a new
perspective and remains unexplored to a large extent.
3. Greywater production, characteristics and reusability aspect
3.1. Greywater quantity
Typical greywater generation rates vary widely from region to re­
gion. Such variations in the order of 20–120 liters per capita per day
(lpcd) is associated with climatic conditions, lifestyle, absorption and
evaporation losses, quality of water supplied, cultural habits and ac­
tivities in the household [26,40]. Table 1 illustrates greywater genera­
tion rates in different countries of the world. It can be comprehended
from the table that the rates differ widely from location to location [27,
Table 1
Rate of greywater production in different countries [27,28].
Location Generation (lpcd)
Africa and Middle East 14–161
Asia 72–225
Gauteng, South Africa 20
Jordan 50
Mali 30
Muscat, Oman 151
Nepal 72
Stockholm 65
Tucson, Arizona (USA) 123
Vietnam 80–110
Calicut, India 79

2
Shreya et al.
28]. Maximum and minimum greywater generation rates corresponding
to high and low-income countries were observed in the USA (Tucson,
Arizona) and South Africa (Gauteng), respectively.
A study conducted by Mandal et al. [29] summarizes the total water
requirements in different activities of an Indian middle-class household
as depicted in Table 2. Quantitatively, it can be assumed that total
greywater generation is approximately 120 lpcd.
3.2. Greywater characteristics
Greywater characterization in terms of physico-chemical and
bacteriological aspect form an important step prior to its reuse. Both the
parameters fluctuate widely because of variations in climate, lifestyle,
cultural habits etc. Approximately, 75% of total water supplied appears
as greywater bearing less number of contaminants as compared to
blackwater [30]. The values of typical parameters of wastewater as
studied by various authors were closely observed and have been sum­
marized in Table 3. Following ranges were found as pH 6.2–9.4,
turbidity 20–444 NTU, TDS 237–2385 mg/L, COD 58–1340 mg/L, BOD
42.1–6250 mg/L, TSS 25–1852 mg/L and surfactant 3–118 mg/L. In
majority of the cases minimal contribution towards pollutant load came
from washbasins and maximum from laundry and kitchen. It is pertinent
to mention that the alkalinity of supplied water influences the pH of
greywater generated [31]. Laundry industry, being a major source of
greywater, generates wastewater with a high pH due to the presence of
alkaline chemicals, which are one of the major ingredients in the form of
detergents [28]. This fact is reinforced by higher pH values observed in
waste streams collected from laundry washing. Cleansing of dirty, oil
stained or infected clothes and shoes in laundry contribute to high fig­
ures of turbidity, COD, BOD, TDS and TSS. It is comprehended from the
table that waste streams from kitchen and laundry have maximum COD
values. The BOD5/COD ratio of greywater was found to vary from 0.31
to 0.71 in an investigation performed by Halalsheh et al. [32]. This
clearly indicates the biodegradable nature of greywater with most of the
biodegradable constituents coming from kitchen waste stream. The
dominance of COD over BOD5 is principally due to presence of recalci­
trant compounds called xenobiotic organic compounds (XOCs) that are
present in a number of household chemicals such as bleaches, surfac­
tants, softeners, builders and beauty products [33]. Eriksson et al. [3] in
their exhaustive study discovered and reproduced a list of 900 different
XOCs present in greywater. However, this study was strictly based on list
of ingredients mentioned on various household chemical products under
survey. Kitchen waste is a primary source of nitrogen in greywater with
a typical range between 4 and 74 mg/L, while detergents used in
washing are the main source of phosphates which range between 4 and
14 mg/L [34]. Phosphate contamination in greywater is chiefly because
of the presence of detergent builders in household chemical products.
These builders (e.g. sodium tripolyphosphate) form an integral part of
detergent formulations [33]. Bathroom and laundry greywater both
were found deficient in nitrogen content [35].
The bacteriological content from different sources displayed wide
variations. Since toilet waste does not mix with greywater, the bacterial
load is lesser in the latter case. Waste streams originating from washing
Table 2
Total water requirements in different activities of an Indian middle-
class household [73].
Sources Water requirement (lpcd)
Hand basin 17
Bath/shower 30
Kitchen 37
Laundry 33
Total greywater 117
Other 23
Toilet flushing 25
Total wastewater 160
3
Surfaces and Interfaces 27 (2021) 101532
nappies and cleaning hands after toilet use contributed largely to fecal
contamination. Poor personal hygiene also plays an important role in
increasing the microbial content of greywater. Studies conducted by
Eriksson et al. [3] revealed a large proportion of excreta-related path­
ogens associated with greywater. Discharge from kitchen also showed
high presence of microbial contamination with Fecal Coliform up to 4 ×
106 MPN/100 mL. This could be attributed to usual raw vegetable and
meat washing. Presence of coliform bacteria and E. coli in greywater is a
definitive and popular way to gage fecal contamination.
3.3. Greywater reuse
Various reuse options like toilet flushing, agricultural purposes,
groundwater recharge, car washing and fire extinguishing have been
explored and proved to be a workable option for reuse [34]. There is no
dearth of techniques (treatment processes) developed to treat the
greywater but unfortunately due to lack of application of such tech­
niques (e.g. dual discharge system), the potential to derive benefits from
treated greywater almost gets attenuated. Treated gray water is widely
reused for a numerous domestic, commercial, agricultural, industrial
and other non-potable uses [36,37]. Greywater stream collected from
bathrooms can be successfully used in toilet flushing systems prompting
reuse and lowering demand for freshwater sources [38]. Prodanovic
et al. [39] tested the possibility of using greywater in green wall systems.
A green wall is a recently developed concept which grows plants in a
media filled planter boxes and is suspended on a side of a building to
give esthetic touch in addition to thermal insulation and benefits like
increased livability and noise mitigation. One dimensional column
studies were made examining the possibility of growing plants by
passing greywater through different viable green wall media e.g.
expanded clay, river sand, perlite, coco air etc.
Many countries such as South Africa, Syria and Australia are utilizing
greywater for gardening purposes. Practice of using untreated greywater
on agricultural land is not uncommon. For irrigation purpose, it has been
noticed that different plants react to application of greywater in
different ways. Studies have found that presence of micronutrients and
macronutrients in greywater increase crop yield of plants like tomato,
silver beet and carrots [40–42]. In general, presence of nitrogen and
phosphorous in greywater act as a good source of nutrients for plant
growth [43]. The possible presence of pathogens, high organic load,
surfactants and suspended solids however limits the opportunity to
reuse greywater. Inhalation of aerosols during application of greywater
on agricultural land may cause problems, hence sub-surface irrigation is
recommended. Direct usage or insufficiently treated greywater if
applied on plants may cause chlorosis i.e. development of brown patches
on the tip of leaves due to accelerated salt levels in the leaves [44]. It is
advisable to store greywater for 24 h as settling of organic material fa­
cilitates improvement in the water quality. However, if the storage
period extends beyond 48 h, drastic level drop in dissolved oxygen leads
to esthetic problems [45]. A study on the effects of treated greywater on
plant growth was made and no adverse impact on soil and plants was
observed. This was mainly due to the reduced concentration of salts,
detergents and minerals post the treatment phase [46]. In case the
greywater is used to irrigate ornamental and food plants, it becomes
imperative to analyze its chemical and microbial characteristics [45].
Therefore, it is necessary to characterize greywater with respect to
physical parameters, as well as the content of both chemical compounds
and micro-organisms before planning for its reuse [3]. Countries such as
Australia, Japan and the USA have released their own greywater reuse
guidelines [47,48]. Some of them offer incentives to encourage its citi­
zens to install greywater treatment systems in their premises while
others have made it a mandatory movement. Most of the standards
developed for greywater reuse have been taken and applied from those
of reclaimed domestic wastewater. Recently, the European Union has
also passed a regulation on the use of reclaimed water. In this regard,
four distinctive classes A, B, C, and D are enlisted for permitted
 Shreya et al.
Table 3
Greywater characteristics.
Greywater pH Turbidity D.O. Phosphate Nitrate TDS COD BOD (mg/ TSS (mg/ Surfactant Ammonia-N Ortho-P FC (MPN Coliform, TC (MPN/ 100 Refs.
source (NTU) (mg/ (mg/L) (mg/L) (mg/ (mg/L) L) L) (mg/L) (mg/L) (mg/L) /100 mL) (MPN/100 mL)
L) L) mL)

Bath/ 7.5 – – – 2.6 277 461 81 148 – 2.1 – 930 – – [105]

shower
Washbasin 7.5 – – – 2.5 237 225 43 48 – 1.6 – 39 – –
Kitchen 6.2 – – – 11.4 245 602 293 308 – 4.7 5.3 230 – –
Laundry 9.4 – – – 79 1060 824 269 1852 – 10.7 18 430 – –
Bath/ 7.6 92 – 1 0.4–0.9 – 424 216 120 – – – 1–2500 – 708,200, 6 × [3]
shower 106
Kitchen – – – 15.6 0.45–5.8 – 936 536 235 – – – – – –
Laundry 8.1 108 21–101 1.6–2 – 725 472 165 – – 728 7 × 105
Shower 7.4 375 2.6 – 28.7 330 294.3 130 353 14.9 – – >200.5 – [118]
Washbasin 7.1 133 3 – 10.2 312 58 42.1 505 41.9 – – >200.5 –
Laundry 8.3 444 2.9 – 25.8 2385 231.3 179.7 315 118.3 – – >200.5 –
Bath/ 7.4 4.9 – – – – – – – – – 1.54×106 – 5.1 × 106 [117]
shower
4

Kitchen 8.3 – 3.5 – – – – 470–4450 – – – – 3.22×106 – 4.3 × 106

Laundry 9.3 – 3.7 – – – – 410–6250 – – – – 2.1 × 106 – 4.2 × 106
Bath/ 7.1–7.4 – – – – – 230–645 173–424 78–303 15–61 0.89–1.2 – 4 × 106 – – [114]
shower
3
Washbasin 7 – – – – – 386 205 259 3.3 0.39 – 3.5 × 10 – –
Kitchen 6.48 – – – – – 1340 890 625 59 0.6 – 1.2 × 106 – –
Laundry 7.5 – – – – 1339 462 188 42 4.9 – 4 × 106 – –
Bath/ 7.3 346 3.6 – 23.6 – 375 380 242 – – – >200.5 – >200.5 [118]
shower
Washbasin 7.2 211 4 – 10.2 – 110 100 318 – – – >200.5 – >200.5
Kitchen 6.7 140 1.4 – 8 – 486 562 134 – – – >200.5 – >200.5
Laundry 8.5 328 3.4 – 16.2 – 471 296 244 – – – >200.5 – >200.5
Mixed 7.3–8.1 – – – – 573 250–375 100–188 100–283 – – – – – – [87]
Mixed 7.3–8.1 20.6–38.7 – – – – 244–284 56–100 – – – – 3.48× – 3.74 × [73]
104–3.56 × 104–3.8 × 104
104
Mixed 6.3–8.1 29–375 100–700 47–466 25–183 0.1–1.5 × 56–8.03×107 [71]

Surfaces and Interfaces 27 (2021) 101532

– – – – – – –
108
Shreya et al. Surfaces and Interfaces 27 (2021) 101532

agricultural use along with the irrigation methods with the major
physico-chemical water quality parameters as E.coli, bio-chemical oxy­
gen demand (BOD5), total suspended solids (TSS) and turbidity [49].
Water reuse guidelines as per different organizations are depicted in
Table 4. It can be inferred from the table that limits on physico-chemical
parameters such as BOD5, total nitrogen (TN), total phosphorous (TP),
TSS, fecal coliform (FC), total coliform (TC) etc. have not been fixed.
This calls for the formulation of a general greywater reuse guideline for
nations who haven’t developed such a protocol till date.
4. Impacts of discharging surfactants in the environment
Instances of polluted lakes spewing froth and creating uncomfortable
conditions in nearby areas have become common. As an example, to
state, Bellandur lake in Bengaluru, India was recently in news for dis­
charging heavy volumes of froth on adjacent roads and residential areas.
It was speculated that indiscriminate usage of large amounts of de­
tergents by households could be the reason for waves of foam formation.
It is interesting to note that though sewage treatment plants help in
reduction of surfactants from raw wastewater, but they leave high
concentrations in sludge that find their way into the environment and
create problems [50]. Common practice of application of sewage sludge
as fertilizer on soil with an aim to replenish its nutrient content may
cause terrestrial toxicity. Strong sorption of surfactants over particulate
matter in sludge leads to accumulation. Though, a large amount of
surfactants produced by industries are biodegradable in nature, their
bulk utilization in higher concentrations has potential to cause severe
damage to the ecosystem [51]. Surfactants can stimulate evolution and
growth of resistant bacterial strains because of their anti-microbial
property. Such mutated microorganisms present in drinking as well as
irrigation water may cause health hazards to human and other living
beings. According to Jensen [52], absorption of surfactant on cell
membrane affect it by causing depolarization of the membrane and in­
hibits micro-organisms to absorb the minerals present in the soil. This
also leads to lower oxygen consumption and decreased cell’s ability to
synthesize toxic metabolic enzymes that subsequently lead to surfactant
build-up.
In rural areas, apparels are washed in open water and the same
surface water is used for domestic purposes. Uncontrolled discharge of
raw sewage from domestic as well as industries into water bodies trigger
aquatic toxicity. Surfactants adsorb strongly on sludge, soil and sedi­
ment, and their sorption follow the sequence of cationic > nonionic >

Table 4
Wastewater reuse guidelines and standards.
ParametersReuse type BOD5(mg/ TN TP TSS pH Turbidity FC TC Residual Detergent Helminth eggs References
L) (mg/ (mg/ (mg/ (NTU) (/mL) (/mL) chlorine (anionic)
L) L) L) (mg/L) (mg/L)

Recreational, ≤10 ≤1.0 ≤0.05 – 6–9 ≤2 ≤10 ≤100 – – – [109]

unrestricted reuse:
lakes and ponds for
swimming;
ornamental fountains;
recreational
impoundments
Recreational, restricted ≤30 ≤1.0 ≤0.05 ≤30 6–9 ≤10 ≤100 – – –
reuse: lakes and ponds
for recreational
purposes without body
contact
Urban, unrestricted ≤10 – – – 6–9 ≤2 ≤10 ≤100 ≤1 – –
reuse: toilet flushing;
laundry; air
conditioning; surface
irrigation of food crops
and vegetables; fire
protection;
construction
Urban, restricted reuse: ≤30 – – ≤30 6–9 – ≤10 ≤100 ≤1 ≤1 –
landscape irrigation;
subsurface irrigation
of food and non-food
crops and vegetables
Greywater for use in NA NA NA NA NA NA NA NA NA NA <1/L, E. [5]
restricted irrigation coli<100,000
(relaxed to
10,00,000 when
exposure is
limited or
regrowth is likely)
Greywater for use in NA NA NA NA NA NA NA NA NA NA <1/L, E.coli<1000
unrestricted irrigation (relaxed to 10,000
of crops eaten raw for high growing
leaf crops or drip
irrigation)
Reclaimed gray water for ≤10 – – ≤10 – ≤10 – – – – ≤10 (number/ [37]
use in agricultural 100 mL), E.coli
irrigation after
secondary treatment,
filtration and
disinfection
Permissible limit for <30 – – – 6–8.5 30 – – – – CPCB-
reuse India

NA: Not Available.

5
Shreya et al.
anionic nature. They are strongly accompanied with soils and sediments,
therefore biodegradation of surfactants is detrimental in determining
their fate in the environment [53]. While average concentration range of
anionic surfactant in domestic wastewater falls between 3 and 21 mg/L,
in many industrial wastewaters it is very high [54]. Trace concentrations
of LAS (an anionic surfactant) in the range of 0.02–1.0 mg/L can damage
fish gills, reduces respiration rate in common goby and alters swimming
patterns in blue mussel larva. Such harmful effects of surfactants on the
environment encouraged various environmental and public health reg­
ulatory organizations to set strict limits on anionic detergent, since its
standard for drinking water is 0.5 mg/L, while up to 1.0 mg/L for other
uses [3].
5. Common methods for treatment of greywater
Aforementioned greywater characteristics suggests for its treatment
prior to reuse. So far, several treatment methodologies have been tried
and tested. All the techniques, in general, can be divided into physical,
chemical and biological processes. Filtration is a simple physical process
wherein the pollutants get trapped inside the pores of a media and
subsequently get removed. Gravel and sand have been found to restrict
the passage of protozoa and viruses, respectively [55]. Various combi­
nations of filter media like pebble, plastic filter, peat, charcoal, bricks,
sand, activated charcoal, polyurethane foam and natural media like pine
bark, coconut shell and coarse sawdust have been tested [46,56,57].
Good removal efficiencies of BOD, TSS and anionic surfactants were
achieved. Use of kenaf dust and chitosan powder to remove common
pollutants like BOD, COD and TSS from greywater was tested by Ridzuan
et al. [58]. Good removal efficiencies of TSS in the order of 90–100%
were obtained. Thirugnanasambandham et al. [59] in their study
explored the use of chitosan to remove BOD and COD from real grey­
water. Chitin from shrimp shells and other marine and terrestrial in­
vertebrates was treated with alkaline substance like sodium hydroxide
to produce chitosan. Apart from being an excellent natural adsorbent, it
also has anti-microbial properties and is easily biodegraded. Under op­
timum conditions, removal efficiencies of BOD, COD and turbidity were
found to be 91%, 73% and 96%, respectively.
Chemical processes such as coagulation and flocculation were tested
using real greywater and high removal efficiencies for BOD (85–88%),
COD (63%), turbidity (88–90%) and PO4-P (95%) were attained [60].
Constructed wetlands (horizontal flow constructed wetlands or vertical
flow constructed wetlands) use plants, a suitable media and microbes to
enhance efficiency of treatment system. It employs physical and bio­
logical treatment processes to treat the wastewater. Studies conducted
by Gross et al. [61], Travis et al. [62] and Arunbabu et al. [63] on
artificial and real greywater reveal high pollutant removal efficiencies
for BOD (>99%), COD (81–95%), turbidity (93%), oil and grease (95%),
PO4-P (67%), NO3–N (98%), TSS (90–98%), Total N (69–82%), Total P
(71%) and anionic surfactants (92–95%). Ramprasad and Philip [64]
focused their research on removal of surfactants in greywater with the
help of horizontal and vertical flow constructed wetlands. Removal ef­
ficiencies of sodium dodecyl sulfate, propylene glycol and trimethyl
amine achieved were 89%, 95% and 98%, respectively. Pathan et al.
[65] investigated the use of rotating biological contactors (RBCs) for
removing BOD, COD and TSS from bathroom greywater. Appreciable
percentage of removal efficiencies were obtained for BOD and COD as 53
and 60%, respectively, but the system could not efficiently remove TSS
(11%). Studies on treatment of greywater (bath, kitchen and laundry)
using RBCs by Kumar and Enayathali [66] was reported to achieve 95%
COD reduction efficiency. Merz et al. [67] examined a laboratory scale
membrane bioreactor (MBR) to treat waste from a sports club. Besides
obtaining an odor free effluent, high removal efficiencies for BOD
(94%), COD (85%), turbidity (98%) and anionic surfactants (97%) were
obtained. The treated effluent met standards for toilet flushing and other
reuse options. A critical review on greywater treatment using MBRs was
presented by Cecconet et al. [68] has proven to provide high quality
6
Surfaces and Interfaces 27 (2021) 101532
treatment to influent wastewater while ensuring efficient removal of
microbes. Such technology can also be provided at decentralized loca­
tions (even at single building site). Bioelectrochemical treatment sys­
tems (BESs) which has developed in the last two decades has been found
to be fitting for treating wastewater that has low organic content. A
common declination of BESs is represented by microbial fuel cells. In
such type of systems, oxidation of organic matter takes place in an
anodic compartment and electrons collected at the anode travel through
resistance to reach the cathode, where they are used in a reduction re­
action. It is a virtually zero-energy input process technology, ideal for
decentralized greywater treatment [69]. Ultra-filtration and nano­
filtration function as very efficient systems for removing BOD, COD,
Turbidity and TSS. Higher permeate quality was obtained from nano­
filtration as removal efficiencies for turbidity and TSS reached an
impressive 98% and 100%, respectively along with the removal of
pathogens like viruses, however cleaning of filters was required at reg­
ular intervals [70]. A sequencing batch reactor (SBR) is a variant of
activated sludge process used for treating wastewater where equaliza­
tion, biological treatment and clarification takes place in only one
reactor. Therefore, the use of separate clarifiers could be avoided.
Different treatment operations are timed controlled. Lamine et al. [70]
studied treatment of shower waste stream using SBR and found high
removal efficiencies for BOD (93%) and COD (80–88%) that easily met
standards for greywater reuse. Anaerobic treatment of greywater was
explored by Elmitwalli and Otterpohl [71] when mixed greywater from
a residential block was treated using upflow anaerobic sludge blanket
reactor (UASB). The slow anaerobic treatment was less efficient in
removing pollutants. The COD, TN and TP removal efficiencies reached
were 52–64%, 22–30% and 15–21%, respectively. Presence of surfac­
tants in high concentrations can drastically reduce methane production
during anaerobic treatment [72]. A study on methods for greywater
treatment and their pollutant removal efficiencies has been summarized
in Table 5.
5.1. Surfactant removal
Greywater is known to cause nuisance principally due to presence of
surfactants or surface-active agents that reduce the surface tension of
aqueous solutions. Shampoos, detergents (for washing laundry and dish-
wares) and other personal care products have surfactants as major in­
gredients. Generally speaking, they can be categorized as ionic and
zwitterionic (amphoteric) surfactants. More than 90% of the ionic sur­
factants produced fall under the genre of anionic or negatively charged
surfactants [3,60]. Greywater commonly inhabit relatively high con­
centrations of detergents prominently containing an anionic surfactant
(29.22%) as sodium dodecyl sulfate (SDS), a non-ionic surfactant (5%)
as propylene glycol (PG), and a cationic surfactant (7.84%) as trimethyl
amine (TMA) along with other constituents. Concentrations of both
anionic and nonionic surfactants below 10 mg/L do not pose harm to
most crops, soils or the environment [73]. In countries like India,
manual washing of clothes is a common practice. Anionic surfactants
like alcohol ethoxysulfates, alkyl sulfates, LAS etc. have excellent
cleansing properties and because of easy availability and affordability,
they find their wide usage especially in low-income households. Present
practices employ use of linear alkyl sulfates in the form of sodium
dodecylsulfate (SDS) because of its biodegradable nature [74]. Schouten
et al. [75] examined the removal of two anionic surfactants viz: LAS and
alpha-olefin sulfonate (AOS) from rinsing cycles of laundry wastewater
through adsorption. Activated carbons synthesized from raw materials
like peat, wood, coconut, bagasse fly ash was also reported in the study.
Apart from the aforementioned natural adsorbents, resins and inorganic
material like bentonite and layered double hydroxide were investigated.
It was gathered that adsorption majorly occurred through ionic in­
teractions between oppositely charged adsorbent and adsorbate sur­
faces. Repulsive forces dominated in case of likely charged species such
as bentonite and cation exchange resins that resulted in minimal
Shreya et al. Surfaces and Interfaces 27 (2021) 101532

adsorption of negatively charged LAS. As compared to micropores (with

[116]
pore diameter <2 nm), mesopores (2–50 nm) and macropores (>50 nm)
Refs.

[43]

[30]
[87]
[89]
[42]

[43]
[10]
[88]
[69]

[75]

[95]
[95]
[70]
[35]
provided favorable site for adsorption of the long (and bigger) chain
molecules owing to their large surface area [76]. Surfactants being large
molecules cannot be captured by micro- porous materials, therefore

>99 (as MBAS)

macro and mesoporous materials are most appropriate for their removal
surfactants

through adsorption [77,78]. Consequently, higher the pore size, pore

Anionic

volume, surface area and porosity higher will be surfactant adsorption.

98.37

92.41

94
95

97
Khan and Zareen [79] studied adsorption of sodium dodecyl sulfo­
–
–

–
–

–
–
–
–
nate (SDS) on granite sand. Ground water was tested in order to judge its
Nitrite

96.92

33.33

applicability on field. Good removal efficiency of the order 70.11% was

100

achieved. The batch sorption studies revealed best adsorption rates at

–

–
–
–
–

–
–

–
–
–
–
highly acidic pH of 2. Langmuir adsorption isotherm model was found as
91–97

15–21
73.68

71.05

18.75
the best fit model which confirmed monolayer adsorption onto the sand
TP

–
–

–
–
–
–

–
–
–
surface. Also, regeneration studies were conducted using hydrogen
peroxide (H2O2) and distilled water as washing agents. In another study,
19–98

22–30
68.51

82.14

62.5

Saleh [80] investigated the use of granular charcoal as a potential

TN

–
–

–
–
–

–
–
–
adsorbent for removal of cetylpyridinium chloride (CPC), a cationic
surfactant from dilute aqueous systems. Adsorption kinetics followed
98.2–100

first order reaction. Studies over pH variations were conducted and it

93.48

89.76

11.08
98.1

43.5
100
TSS

90

was reported that no significant effect on adsorption could be observed.

–

It was concluded that π-π interactions could be considered to be oper­

NO3–N

ating between CPC (carrying pyridine ring) and granulated charcoal.

48.57

The type of mass transfer was found to be dependent on shaking speed-

75

98
–

–
–

–
–

–
–

–
–
–
–

lower speed controlled the rate of external mass transfer (i.e. between
94.58

solution and particles) and higher shaking speed was responsible for
PO4-

67

internal and surface adsorption. Experimental data revealed with in­

P

–
–

–
–

–
–
–
–

crease in temperature, adsorption also increased which pointed towards

95.45
O&G

the chemical or endothermic nature of adsorption. Effect of temperature

98
–

–
–

–
–
–

–
–

–
–
–
–

variations on adsorption characteristics could also be supplemented by

the fact that higher temperature encouraged surfactant micelles to break
TDS

81
–

–
–

–
–
–
–

–
–

–
–
–
–

into monomers and thus become free and available for adsorption. Free
energy, a thermodynamic parameter was calculated and found to have a
Turbidity

high negative value which indicated favorable and strong adsorption

88–90

92–97
98.28
99.92

98.1

onto granulated charcoal. Regeneration studies were conducted by

93
–

–
–

–
–

heating the adsorbent in an oven at 180 ◦ C for 4 h. Granular charcoal

Removal efficiency (%)

45–70

80–88
52–64

was found to possess good removal efficiency post the regeneration step.
81.29

82.16

95.07

99.19
COD

93.3
91
63

95
60

85

Recently, Bolognesi et al. [81] reported the synthesis of biochar from

–

sewage sludge and microalgae and suggested the possible use of it for the
93.7–99.6

removal of various contaminants and a possible role in circular

85–88
99.85

99.22

92.78

economy.
BOD

98

53

94

Bottle adsorption studies on removal of two typical cationic quar­

–

–
–

ternary amine surfactants viz: dodecyltrimethylammonium bromide

Rotating Biological Contactors
Rotating Biological Contactors
Different methods for treatment of greywater and their removal efficiencies.

Coagulation and flocculation

(DTAB) and hexadecyltrimethylammonium bromide (HTAB) over

Sequencing batch reactor

treated and untreated sepiolites or magnesium hydrosilicate was con­

Upflow anaerobic batch
Membrane bioreactor
Membrane bioreactor
Constructed wetlands

Constructed wetlands
Constructed wetlands

ducted by Sabah et al. [82]. Sepiolites, a natural clay minerals are

Treatment technique

known to possess a deep fibrous structure where different ions can

Nanofiltration
Ultrafiltration

penetrate into its interior channels and as a result get separated from the
bulk solution. Adsorption was initially driven by ion-exchange process
Filtration

Filtration
Filtration

reactor

between ammonium ions and magnesium ions in the octahedral layer.

Later hydrophobic interactions amongst adsorbed surfactant molecules
also became prominent which further helped in removal of the pollut­
ants. Even though there was a phenomenal increase in the surface area
of acid treated sepiolites, the adsorption rates plummeted. This was
Mixed- Laundry, bath,

Mixed- Laundry, bath,

Mixed- Laundry, bath,

Mixed- Laundry, bath,

Mixed- Laundry, bath,

Bathroom, washbasin

attributed mainly due to collapse of octahedral sheet responsible for

Bathroom/ Shower
Greywater source

holding magnesium ions in the latticework post the treatment step.

Similar adsorption studies on the removal of SDS and sodium dodecyl
Bathroom

benzene sulfonate (SDBS) were made using Mobil Composition of

Shower

Shower
Shower
Shower
kitchen

kitchen

kitchen

kitchen

kitchen

Matter-41 (MCM-41- a mesoporous material having high surface area)

and activated carbon cloth, respectively [83,84]. Electrostatic in­
–

–
–

teractions between activated carbon cloth and SDBS played governing

role behind the removal process.
greywater

Synthetic
Synthetic
Artificial

5.2. pzc and its importance

Type of
Table 5

Real

Real
Real
Real

Real
Real

Real
Real

Real
Real
Real
Real

Point of zero charge (pzc) is the pH at which the surface of adsorbent

7
Shreya et al. Surfaces and Interfaces 27 (2021) 101532

possesses a net neutrality condition, i.e. surface contains equal number

of positive and negative charges. Below this value, the surface is posi­
tively charged and beyond this value it becomes negatively charged. It is
a fact that cations are easier to adsorb on a negatively charged surface
and anion on a positively charged surface. The pzc of materials can be
commonly determined by means of following four techniques: common
intersection point (cip), isoelectric point (iep), acusto (here, iep is
determined with the help of electroacoustic method) or pH [85].
Charged surfactants adsorb onto solid surfaces chiefly via electrostatic
interactions. The point of zero charge (pzc) is an important aspect that
needs to be considered during adsorption of charged species. Silica is
negatively charged over a wide pH range (pzc of silica~1.7–3.5) and
hence the surface provides unfavorable conditions for adsorption of
anionic surfactants. Rock-sandstone reservoirs are primarily composed
of silica and therefore it is advantageous to use anionic surfactants in
such strata. Some clay minerals like kaolinite and illite lack homogenous
surface and as a result adsorb anionic surfactants. Adsorption studies of
surfactants over carbonate materials such as dolomite, limestone, calcite
and silica were investigated. Natural dolomite was found to possess
divalent ions such as Ca2+ and Mg2+ that repelled cationic surfactants Fig. 1. Schematic representation of typical four regime adsorption isotherm
and instead adsorbed anionic surfactants. Pure limestone adsorbed (adopted from [86]).
anionic surfactant (SDS) more efficiently than cationic surfactants such
as cetylpyridinium chloride (CPC) and dodecylpyridinium chloride interaction between the adsorbed monomer. Such lateral interactions
(DPC). In addition, it was highlighted in the study that if impurities like between hydrocarbon chains lead to surface aggregation (cluster for­
silica and aluminum were present in limestone, the negative charge mation) called hemi-micelles and they are formed beyond a certain
developed as a result would repel SDS and favor adsorption of cationic concentration below CMC. When surface of adsorbent is electrically
surfactants. Similarly, pure calcite that had abundant Ca2+ ions showed neutralized by adsorbed surfactant ions, there is a marked decrease in
higher affinity for SDS than CPC mainly because of the electrostatic adsorption. The electrostatic forces weaken in this region and adsorption
attraction. Mineral constituents of natural carbonate materials vary take place via lateral interactions only (Region III). In region IV the
widely and hence non-uniform adsorption behavior was observed. In a adsorption remains constant and any further addition of surfactant lead
nutshell it could be inferred that adsorption of cationic or anionic sur­ to micellization. It was also highlighted that an increase in temperature
factants was favored depending upon the purity of the carbonate ma­ increased kinetic energy of surfactant molecules, which led to decrease
terial. The surface charges (electrostatic) present on the adsorbent also in adsorption of sodium dodecyl sulfate over a clay surface.
determines the efficiency of different types of surfactants, which can be An analogy can be derived from studies conducted by Adak et al. [3]
controlled by pH of solution. For effective adsorption of anionic sur­ wherein adsorption of SDS over neutral alumina has been well explained
factants, positive superficial charge on the adsorbent is appropriate, diagrammatically. Fig. 2 shows how at low SDS concentration the
while negatively charged adsorbent surface is required to adsorb monomers are formed at the surface and upon further increase in the
cationic surfactant. However, adsorption of nonionic surfactant neces­ surfactant concentration monolayer structure called hemi-micelle and
sitates the nonpolar adsorbent, while both positive and negative charged bilayer structure called admicelle are formed.
adsorbents are suitable for amphoteric surfactants. The hydrophobicity of adsorbents also helps in the adsorption of
surfactants and adsorbents with higher hydrophobicity adsorb higher
5.3. Mechanism of surfactant adsorption quantity of surfactants and vice versa. Mechanically stability of adsor­
bent at environments of strong acids and alkalis and high temperatures
Surfactant adsorption over solid surface is generally said to follow a and pressure is very important. The eco-friendly and economical
two-step approach viz: electrostatic attraction between surfactant and
adsorbent; and hydrophobic or tail-tail interactions between surfactant
molecules (Zhu and Gu, 1991). Mechanism behind surfactant adsorption
over solid surfaces in aqueous medium has been studied by various
authors. Zhang and Somasundaran [86] established that ionic surfac­
tants adsorb onto oppositely charged solid surface followed “Soma­
sundaran–Fuerstenau” type isotherm. The isotherm was chiefly
characterized by electrostatic attraction at low surfactant concentrations
and electrical double layer formation over the solid surface at concen­
trations above critical micelle concentration. Similar facts of electro­
static and lateral chain-chain interactions were portrayed by Paria and
Khilar [87] and they listed following possible adsorption methods-
ion-exchange, ion-pairing, hydrophobic interactions, polarization of
electrons and Van der Waals forces. Fig. 1 shows a four-region adsorp­
tion isotherm for surfactant adsorption over cellulose surface. Cellulose
is a natural, renewable and biodegradable material that has a good
potential of being utilized as an adsorbent for eliminating pollutants like
phenols, dyes, pesticides, metals etc. from water [88]. Region I occurs
when surfactant concentration is low, and monomers are electrostati­
cally adsorbed to the adsorbent. The region obeys Henry’s law and in­
creases linearly with increase in surfactant concentration. In region II,
there is a sudden rise in adsorption which can be attributed to lateral Fig. 2. Formation of bilayer of SDS on alumina surface (adopted from [3]).

8
Shreya et al.
adsorbents are preferable for surfactants removal [89].
Surface solubilization is a concept put forth by Stigter et al. [90] and
during their experimentation work they explained the solubilization
phenomenon as co-adsorption of Orange OT (dye) with lauryl­
trimethylammonium chloride (a cationic surfactant) over glass surface.
A study using mixture of Chrome Azurol S (CAS, an anionic dye) and
three non-ionic surfactants and their adsorption over silica gel was made
by Zhu and Gu (1991). The test revealed following interesting results-
solution of the anionic dye alone displayed a yellow color and when
surfactants were added, the color of remained unchanged but when
concentrations of surfactants increased above their critical micelle
concentration (CMC), color transformation from yellow to dark red
occurred. This was because of solubilization of CAS into micelles. A
coherent study on CAS adsorption over silica gel was made. The color of
silica gel in the solution appeared as light yellow but as non-ionic sur­
factants (below their CMC) were introduced into the system, light or
dark red color appeared. It was comprehended that due to adsolubili­
zation, a micro-environment developed over the adsorbent surface
which imitated micelle formation in bulk solution and hence explained
the color change.
Removal of organic pollutant along with cationic surfactants through
adsolubilization was reported by Koner et al. [91] during their studies
on silica gel waste as potential adsorbent for removing cationic surfac­
tant from industrial wastewater. At lower concentrations the surfactants
formed hemimicelle (or monolayer) on the solid surface but at higher
concentrations (above CMC), admicelle (or bilayer) formation occurred
owing to hydrophobic interactions between cationic surfactants. Adso­
lubilization of dyestuffs between these hemimicelles or admicelles hel­
ped in their removal. Fig. 3 illustrates the adsolubilization process
wherein dye molecules solubilize within the hemimicelle or partial
admicelle.
Da˛browski [92] published studies on kinetics and dynamics of
adsorption and indexed following stages in adsorption kinetics (a time
dependence phenomenon) as - external, internal and surface diffusion.
Internal diffusion referred to transfer of molecules from bulk to
solid-liquid interface. Diffusion of adsorbate inside the pores of adsor­
bent was termed internal diffusion. Surface diffusion incorporated the
concept of molecule transfer in the surface phase.
5.4. Removal of surfactants through adsorption
Diverse alternatives for treatment of wastewater are available and
each have their benefits and drawbacks. There exist different conven­
tional methods viz: coagulation [93], electro-coagulation [94] and
membrane separation [95] for removal of surfactants. Such methods
involve high operational and maintenance costs and an added burden of
disposing toxic sludge into the environment. Among all the alternatives,
adsorption holds a promising future. Drugs, surfactants, pharmaceuti­
cals, personal care products have been in focus as they are emerging
pollutants in the terrestrial and aquatic environment. Their production
and usage are gradually on the rise. A summary of adsorbents used for
removal of pollutants is given in Table 6.
In recent years, a number of studies have been made using
Fig. 3. Schematic representation of adsolubilization process (adopted
from [66]).
9
Surfaces and Interfaces 27 (2021) 101532
lignocellulosic precursors, biomass sources and agricultural waste as
adsorbents and their conversion to activated carbon through chemical or
physical activation [96–98]. The application of adsorbent materials such
as stems of plants, shells, fibres, fruit/vegetable peels [99], seeds, husks,
wood, waste materials etc. have been identified as possible potential
adsorbents for removal of heavy metals, dyes [100], phosphates [101],
fluoride [102], antibiotics [103] volatile organic compounds etc. The
studies have indicated lignin as the primary component in lignocellu­
losic biomass responsible for carrying out the process of adsorption.
Materials with high lignin, carbon and volatile matter content and less
ash content pose as good adsorbents [41].
Adsorptive removal of anionic surfactant (SDS) from laundry
wastewater over alumina was investigated by Adak et al. [3]. Both batch
and column studies were performed where SDS removal followed
pseudo-second order reaction kinetics and produced 94% removal effi­
ciency at optimized conditions. Natural pH of the wastewater was found
to be 9.1 and because the pzc value of alumina was 9.15, the pH of
wastewater sample was brought down to 5.5 for effective removal of the
pollutant. This enhanced electrostatic attractions between more posi­
tively charged alumina and negatively charged surfactant. Similar
studies have been conducted in order to study better removal effi­
ciencies by adjusting solution pH [104]. It is to be pointed out that
hydrophobic (chain-chain) interactions between surfactant molecules
also played an important role in the adsorption process. The lateral in­
teractions between hydrophobic tails of surfactant molecules increased
because of the presence of total dissolved solids (TDS). This was
reportedly due to decrease in lateral repulsive forces between charged
head groups of ionic surfactants which subsequently led to increase in
adsorption.
Waste activated carbon from water purifiers was tested for removal
of SDS through adsorption by Gupta et al. [45]. Under optimized con­
ditions waste activated carbon (with particle size in the range of
1000–500 μm) was shown to remove up to 98% of SDS. An ultrasonic
cleaner (for the purpose of sonication) was employed for desorption and
regeneration of exhausted waste activated carbon. Energy dispersive
spectrometry studies confirmed the adsorption of SDS when the sulfur
content increased from 30 to 60% during pre and post adsorption,
respectively. Langmuir model was found to fit best during the adsorption
isotherm studies and maximum adsorption capacity was evaluated as
61.35 mg/g with initial SDS concentration of 15 mg/L. Another study on
SDS removal over waste tire rubber granules was conducted by Pur­
akayastha et al. [105]. The adsorption process was found to be film
diffusion controlled. High percentage removal efficiency of 92 was
achieved. Langmuir adsorption isotherm fitted best giving maximum
adsorption capacity as 4.16 mg/g.
Removal of cationic surfactant from textile wastewater using silica
gel waste (with silica content as 96%) as adsorbent was examined by
Koner at al. [106]. Adsorption studies were found to follow Freundlich
isotherm model achieving 87% removal efficiency under optimized
conditions. In addition to adsorption of cetyltrimethylammonium bro­
mide, a cationic surfactant tested in the study, removal of other organic
pollutants from the wastewater sample was also observed. These or­
ganics were found to be subsequently removed along with the ionic
surfactant through a process called adsolubilization. The observance
was supplemented by the fact when approximately 81% color reduction
was noted. Good color removal efficiency was detected mainly due to
adsolubilization of dyestuffs, an organic pollutant, within the surfactant
molecules. During comparative studies made between removal effi­
ciencies of the cationic surfactant from real wastewater and cationic
surfactant spiked distilled water (both having same initial concentration
and adsorption conditions), it was established that the former case bore
higher removal statistics. Interestingly the obtained results were
attributed to presence of higher TDS that weakened the electrostatic
repulsion between adjacent adsorbed surfactant molecules. Moreover, it
was gathered that real wastewater sample had higher pH (9.2) than
distilled water (near neutral) and as pzc of adsorbent was found to be 2,
Shreya et al. Surfaces and Interfaces 27 (2021) 101532

Table 6
Removal of surfactant through adsorption.
Name of Adsorbent Compound removed Mode of Dependent parameters Removal Adsorption Refs.
operation Concentration pH Temperature efficiency Isotherm
( ◦ C) (%)

Alumina SDS Batch and 8068 mg/L 5.5 Room 94 – [3]

column temperature
Waste Activated SDS Batch 10–20 mg/L 3–10 30 71–73 Langmuir [45]
Carbon
Waste tire rubber SDS Batch 4–10 mg/L 6 Room 92 Langmuir [93]
granules temperature
Activated carbon SDS Batch 5 mg/L 8.6–10.2 Room 57–95 – [18]
(AC) temperature
Granular charcoal Cetylpyridinium chloride Batch – 2,6.8,11 30–60 98 Modified [101]
frumkin
Silica gel waste Cetyltrimethylammonium bromide Batch and 362 mg/L 9.2 15–35 87 Freundlich [66]
(SGW) column
Lagenaria vulgaris SDBS Batch 10–1200 mg/dm3 1–9 Room 99 Langmuir [33]
shell temperature
Copper Anionic detergents- SDS and SDBS; Batch Anionic detergents- 2–8 30–45 80 (SDS) Langmuir [115]
Ferrocyanide Cationic detergents- Cetylpyridinium 10− 5 to 10− 6 M;
bromide (CPB) and Cationic detergents-
Cetyltrimethylammonium bromide 10− 4 to 10− 5 M
(CTAB)
Rice husk Anionic surfactants (AS)- LAS and alkyl Batch and AS- 1, 10 and 100 2–6 (for Room AS- 97; – [57]
phenol ethoxylates; non-ionic column mg/L; NPE- 10–80 AS) and temperature NPE- 75
surfactant- nonyl phenol ethoxylate mg/L 2–10 (for
(NPE) NPE)
Agricultural (stems LAS Batch 25–100 mg/L – Room Leaves- 40; Leaves- [14]
and leaves) and temperature Stem- 33 Freundlich;
agro-industrial Stems -
(hod and cob) Langmuir
corn residues
Coconut shell SDBS Batch 15–45 mg/L 2–12 20–50 93 Langmuir [16]
Chitosan hydrogel SDS Batch 10–60 mg/Ls 5–11 Room 99 Langmuir [85]
beads temperature
Dolochar SDS Batch 50 mg/L 2.4 Room 99 Langmuir [112]
temperature

the adsorbent particles became more negative which boosted the
adsorption rates. Regeneration studies were successfully conducted
using dilute hydrochloric acid (pH < 1).
Adsorption of SDS over activated carbon was studied by Bindes and
Franco [107]. Four different sizes of activated carbon (using mesh sizes
400, 200, 100 and 60) were investigated. Better removal efficiencies
were obtained for adsorbent sizes above mesh 200 and having small
pore diameter of 0.56–0.77 nm. Surfactant removal efficiencies were
found to vary between the range 57–95% with electrostatic and hy­
drophobic interaction acting as major forces of adsorption. Another
study on adsorption over metal oxide surfaces was conducted in the
presence of both anionic and cationic surfactants in aqueous system by
Upadhyaya et al. [108]. It was gathered that upon addition of cationic
surfactants- dodecylpyridiniumchloride (DPCl) and benzethonium
chloride (BCl) over pre-adsorbed alumina surface with anionic surfac­
tants- sodium dihexyl sulfosuccinate (SDHS) and SDS, the adsorption
enhanced. Inclusion of DPCl and BCl between oppositely charged SDHS
and SDS over adsorbent surface led to decrease in electrostatic repulsion
between similar charged anionic head groups which brought them
closer following dense packing that eventually explained the unexpected
rise in adsorption. Similar developments were noticed when adsorption
study of SDS over pre-adsorbed silica (having negatively charged sur­
face) with DPCI was made. Also, it was observed that while DPCI
wouldn’t adsorb on positively charged alumina alone, but it readily
adsorbed over pre-adsorbed alumina with SDS. Electrostatic attraction
between oppositely charged SDS and DPCI head groups brought about
co-adsorption of DPCI in conjunction with SDS on alumina.
Another study on adsorption of SDS using chitosan hydrogel beads
was conducted by Pal et al. [85]. The removal efficiency was ~65% in
first 24 h but it reached an impressive ~99% on fifth day. The kinetic
data revealed pseudo-second order rate was followed best. The main
mechanism behind SDS adsorption could be attributed to electrostatic
interactions between chitosan and SDS. The research further revealed
that since SDS adsorption over chitosan hydrogel beads was indepen­
dent of pH variation (5.0–11.0), hydrophobic interactions between the
hydrophobic functions of the adsorbate and the adsorbent molecules
must have played an important role along with the ionic interactions.
Similarly, Shami et al. [109] utilized dolochar as industrial waste
product for removal of SDS from aqueous solution in batch as well as
column mode. Authors reported 99% of SDS removal efficiency at an
adsorbent dose of 16 g/L maintaining an optimum pH of 2.4. Out of
several tested isotherms, Langmuir was appeared as best fit producing
an adsorption capacity of 5.78 mg/g at optimized condition. Further, a
bed depth service time (BDST) model was applied to verify the column
performance, and to scale up the process parameters. This study
demonstrated the meaningful and sustainable use of industrial waste
material to protect the environment.
5.5. Use of low-cost natural adsorbents
Chemically modified Lagenaria Vulgaris shell (lignocellulosic
biomass) was tested for adsorptive removal of SDBS by Velinov et al.
[110]. Adsorption studies pointed towards Langmuir adsorption model
as the best fit indicating monolayer type of adsorption and maximum
adsorption capacity was calculated as 513.28 mg/g. Scanned electron
microscopy (SEM) revealed porous (macropores) nature of the bio­
sorbent. It was observed that chemical treatment with Al2O3 brought no
significant changes in the structural morphology. Examination through
energy dispersive X-ray spectroscopy (EDX) of modified biosorbent
found a slight increase in its oxygen content. Fourier transform infrared
(FTIR) spectroscopy revealed a possibility of –OH group behind the
sorption process. Varying pH from 1 to 9 exhibited a decreasing trend in
the removal efficiency of the anionic surfactant. Positive charge on
adsorbent and negative charge possessed by sulfonate groups of SDBS

10
Shreya et al.
may explain the ion-exchange phenomenon majorly responsible for
adsorption. But as pH of the medium increased beyond pzc of the
adsorbent (which was 5.85), the adsorption rates plummet sharply and
reached minimum at pH 9. It was inferred that due to low-cost, high
mechanical stability and easy availability, the modified biosorbent holds
good scope for removal of anionic pollutants from water.
Removal of anionic surfactants- LAS and alkyl phenol ethoxylates
and non-ionic surfactant- nonyl phenol ethoxylate on rice husk was
investigated by Hosseinnia et al. [111]. Percentage removal was calcu­
lated as 97 and 75 for anionic and non-ionic surfactants, respectively.
Increase in removal efficiency at acidic pH was noted for the anionic
surfactants. This was chiefly due to adsorption of sulphonic group in its
acidic form over the rice husk. For non-ionic surfactant, adsorption
trend did not show any variation with changing pH because of the
non-ionic nature of nonyl phenol ethoxylate. Adsorption was said to take
place via Van der Waals forces operating between surfactants and the
cellulosic layer of rice husk.
Batch adsorption studies for the removal of LAS from greywater
using agricultural waste were conducted by Tejada-Tovar et al. [112].
Leaves, stems, cob (usually a green covering that wraps the corn) and
hod (cylindrical part over which corn grains are secured) of corn as
agricultural residues were employed as adsorbents in the study. Stem of
corn produced the superior LAS removal efficiency over leaves. Chem­
isorption (as removal mechanism in corn leaves) was found to operate
via transfer of electrons between the adsorbate and adsorbent.
Elemental analysis of all four biosorbents showed stem had maximum
proportions of lignin, cellulose and hemi-cellulose which probably
explained why it exhibited best adsorption characteristics. Adsorption
studies revealed corn leaves obeyed Freundlich isotherm (multi-layer
adsorption) and corn stems followed Langmuir adsorption model
(mono-layer adsorption). Adsorption kinetics reported pseudo-second
order and intra-particle diffusion model as best fits for corn leaves and
stems, respectively.
Coconut shell after its thermo-chemical and chemical activation was
tested for adsorptive removal of SDBS by Bhandari and Gogate [113].
Adsorption kinetics was found to follow pseudo-second order model.
Study revealed excellent adsorption at a pH of 2 (pzc of the adsorbent
found to be between 2 and 3) and minimum at pH of 12. Presence of
hydroxyl ions (OH− ) at higher pH led to increased competition with the
anionic surfactant molecules for adsorption over coconut shell which
explained the observed trend. It was comprehended that lateral hydro­
phobic and electrostatic forces were the reason behind enhanced
adsorption at lower pH. The adsorbent was regenerated via gentle
washing, heating at a temperature of 110 ◦ C for 3 h and later soaking it
in distilled water having high alkalinity. Escalated negative values
observed for thermodynamic parameters revealed high spontaneity,
decrease in randomness and exothermic nature of adsorption.
6. Future prospective
Removal of some of the recalcitrant and toxic compounds like sur­
factants, detergents has been the focal point of the study and a research
on finding the optimum low-cost adsorbents that could remove such
pollutants should be investigated. Further, depending upon the type of
contaminant, the low cost adsorbent mainly the waste materials may be
modified to improve their adsorption capacities. This could greatly help
in the conservation of water at a household or community level. Efforts
may be made to conduct the risk assessment, comparative cost analysis
related to the adsorptive removal of surfactants from gray water and
regeneration of adsorbents.
7. Conclusion
This paper underlines the removal of surface-active agents and
related compounds from greywater using low-cost adsorbents. In the
current review, not many studies could be found in relation to treatment
11
Surfaces and Interfaces 27 (2021) 101532
of greywater using low-cost natural adsorbents, thus, the area holds a
bright scope for development in the near future. In order to determine
the most effective adsorbent, it calls for a close examination of various
alternatives. Removal of recalcitrant and toxic compounds along with
BOD and microbial reduction should be gauged. Greywater generally
contains high concentrations of easily biodegradable organic materials
and some basic constituents that are largely generated from households.
With an aim to utilize adsorbents originated as waste from different
industrial sectors not only reduce the cost of treatment but also put the
hugely generated scrap to a better use. In order to reduce our increasing
dependency on depleting fresh and groundwater sources, it has become
imperative to opt for greywater reuse. Such adsorbents can be used to
design simple adsorption units at household level, thereby increasing
local level participation and reducing stress on central wastewater
treatment facilities. The treated water can be utilized for a number of
non-potable purposes. Adsorption processes for removing pollutants
from greywater is a very cost-effective technique. Low-cost adsorbents
are cheap and affordable. It prevents unnecessary disposal of products
that can be put to best use especially in conserving water, a precious
resource. Moreover, maximum benefit can be attained if employed in
rural areas of developing nations like India.
Declaration of Competing Interest
The authors declare no conflict of interest.
Acknowledgments
The authors wish to acknowledge the Department of Civil Engi­
neering and Bio-fuel & Bio-processing Research Center, Siksha ‘O’
Anusandhan (Deemed to be University), Bhubaneswar and School of
Infrastructure, Indian Institute of Technology Bhubaneswar for facili­
tating the research work.
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