Cleaner Engineering and Technology 4 (2021) 100209

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Cleaner Engineering and Technology

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A critical review of biosorption of dyes, heavy metals and metalloids from

wastewater as an efficient and green process
A.M. Elgarahy a, K.Z. Elwakeel b, c, *, S.H. Mohammad a, G.A. Elshoubaky d
a
Zoology Department, Faculty of Science, Port-Said University, Port-Said, Egypt
b
University of Jeddah, College of Science, Department of Chemistry, Jeddah, Saudi Arabia
c
Environmental Science Department, Faculty of Science, Port-Said University, Port-Said, Egypt
d
Botany Department, Faculty of Science, Suez Canal University, Ismailia, Egypt

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

Keywords: Wastewater contains many organic and inorganic pollutants and discharging them into received waters leads to
Biomass serious environmental problems. The wastewater that is produced from various industries contains a noticeable
Biosorbent amount of dyes; heavy metals and metalloids this has remained one of the major environmental problems facing
Dyes
public health. Unfortunately, the conventional wastewater remediation process is unable to remove dyes and
Heavy metals
Remediation
heavy metals completely. One of the widely used water treatment technologies is biosorption, biosorbents are
Wastewater considered to be an emerging green, cost-effective, and efficient alternative. Therefore, the search for locally or
regionally available biomasses for heavy metals/metalloids and dyes removal gained rapid attention. Methylene
blue, Crystal violet, Reactive black 5, and Congo red; Cd, Cr, Cu, Pb, Hg, Ni, and Zn; and As were selected as
examples for dyes, heavy metals, and metalloids, respectively, In this regard, a comprehensive understanding of
the biosorption capability of different biosorbents is necessary to know how they can remove inorganic and
organic contaminants in wastewater. Biosorption is an ion exchange, complexation, and coordination process.
Besides, the recent advances in various biomaterials-based biosorbents and different approaches of pollutants
removal from wastewater with several examples to provide a backdrop for future research have been reviewed.
This can be beneficial for developing more effective technologies to eliminate contaminants, thus bridging the
gap between laboratory results and industrial use. crustacean shells, algae, chitosan are the most effective bio­
sorbents. These biosorbents can serve as good alternatives to synthetic materials for pollutants removal from
wastewater.

1. Introduction development. Many types of industries such as machinery

Water is the greatest gift from nature because of its indispensable
importance for the survival of different biota on our planet (Mikosch
et al., 2020). As it is one of the finite natural resources, maintaining its
quality is a global demand that extensively increases with each passing
day. Regrettably, in the new millennium, many crises, conflicts, and
wars on limited water resources have emerged. Also, different water
pollutants are related to innumerable human activities being synchro­
nously emitted into water bodies causing severe declination in water
specifications (Richa and Roy Choudhury, 2020). Agricultural, com­
mercial, domestic and industrial sectors will suffer from clean water
scarcity. The current and next generations will pay a huge price as a
result of an acute contradiction between limited resources and economic
manufacturing, printing, textile (Yao et al., 2020), chemicals, elec­
tronics, and pharmaceutical industries are implicated in water pollution
(Özdemir et al., 2019). They are responsible for the seepage of different
pollutants such as dyes (Tonato et al., 2019), heavy metals, phenols
(Mohammed et al., 2018), pesticides (Behloul et al., 2017), insecticides,
and drugs (de Lima et al., 2018) into the aquatic environment as
byproducts without proper manipulation. The presence of pollutants in
water bodies above their allowable levels set by the World Health Or­
ganization (WHO) and Environmental Agencies may have tremendous
effects (Nishikawa et al., 2018). These effects can impair human and
animal health (neural toxicity, carcinogenicity, and reproduction ca­
pabilities) (Fontana et al., 2018). It also may result in eutrophication and
photosynthesis inhibition (Aboelfetoh et al., 2018). This was due to its

* Corresponding author.University of Jeddah, College of Science, Department of Chemistry, Jeddah, Saudi Arabia.
E-mail addresses: Khalid_elwakeel@yahoo.com, Khalid_elwakeel@sci.psu.edu.eg (K.Z. Elwakeel).

https://doi.org/10.1016/j.clet.2021.100209
Received 12 November 2020; Received in revised form 17 June 2021; Accepted 2 July 2021
Available online 4 July 2021
2666-7908/© 2021 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
A.M. Elgarahy et al.
poor degradability and/or highly accumulating effects (Novais et al.,
2018).
Both dyes and heavy metals are conceived to be some of the most
dangerous pollutants in water systems as they exhibit mutagenic,
immunogenic, carcinogenic, and teratogenic characteristics (Azari et al.,
2019). Discharge of wastewater into aquatic bodies without proper
purification causes numerous significant environmental and health
problems for aquatic flora, fauna, and finally human health (Yin et al.,
2019).
Dyes can be categorized into three main groups: (a) anionic (acid,
reactive, and direct dyes) with negative charge mainly due to (SO3− )
group, (b) cationic (basic dyes) due to the protonated amine group, and
(c) nonionic (disperse dyes) according to their dissociation behavior in
aqueous solutions (Sakin Omer et al., 2018). Azo dyes either cationic or
anionic bear one or more azoic bonds (N– – N). Besides its stability
against light, heat, and aerobic digestion, it may cause severe threats to
human health such as vomiting, cyanosis, allergic problems, and genetic
mutation. The dye industry gives emblematic examples of the potential
impact of uncontrolled management of contaminated flows (Pellicer
et al., 2018). Dyes are used in a great diversity of sectors: textile, paper,
leather, dyestuff, printing, plastic, cosmetics, and coatings which are
widely disseminated because of low-cost production, brightness, and
high resistance against environmental conditions (Reck et al., 2018).
Even at low concentrations, dyes are optically active and detectable
(Bello et al., 2018); their impact on water bodies is then very acute (dos
Santos et al., 2018). Indeed, the dispersion of dyes in water assets dis­
turbs gas solubility, which, in turn, affects the gills of aquatic organisms
and disrupting their spawning sites and refuges (Senthil Kumar et al.,
2018). While hindering light penetration in water, the dyes also limit
photosynthesis. Apart from these secondary effects, the dyes have
frequently specific toxicity due to carcinogenic and mutagenic effects
(associated with the presence of benzidines, and naphthalenes de­
rivatives) (Pleşa Chicinaş et al., 2018).
Heavy metals are inorganic notorious contaminants that are defined
as chemical elements with relatively high atomic weight and density. It
is poisonous even at low concentrations (Ali et al., 2019). Massive
amounts of toxic metals like As(III), Cd(II), Cu(II), Cr(VI), Ni(II), Pb(II),
and Zn(II) are dumped into water assets without proper treatment
(Dobrowolski et al., 2019). These pollutants in waterways represent a
serious threat (Que et al., 2019).
Owing to the mentioned discredited impacts on different biota, a
strong demand for water purifying from dyes and heavy metals becomes
a paramount need. It is an important issue for the industry, the envi­
ronment, and health. Physical, chemical, and biological approaches are
implemented to capture it from water systems. Physical and chemical
processes include coagulation/flocculation (Hou et al., 2019), precipi­
tation (Chen et al., 2018), ion exchange (Feng et al., 2019),
photo-oxidation (Du and Chen, 2018), electrocoagulation (Doggaz et al.,
2019), electrodialysis (Nemati et al., 2017), membrane separation
(Hosseini et al., 2018), ultrafiltration (Kavitha et al., 2019), forward
osmosis (Qiu and He, 2019) and irradiation (Ghobashy and Elhady,
2017), and adsorption (Wei et al., 2021). Whilst the biological processes
include phytoextraction (Napoli et al., 2019) and biological degradation
(Jacob et al., 2018). Figure S1 (see supplementary material) presents the
conventional wastewater treatment processes in more detail.
However, most of these sophisticated processes have many certain
limitations. They are high costs, inefficiency in low pollutant concen­
trations, huge time consumption, reagents and energy, and chemical
sewage sludge formation (Fernando et al., 2018). It is time to come up
with an alternative, greener, and cheaper technology for the efficient
elimination of different contaminants from water (Hadiani et al., 2019).
Consequently, exploring an efficient route for dyes and heavy metals
elimination remains a great challenge. It is a bottleneck for preserving
water resources. Recently, Researchers have assessed several bio­
materials for the remediation of contaminated effluents in the quest for
environmental protection and sustainability. For example, Ubando et al.
2
Cleaner Engineering and Technology 4 (2021) 100209
conducted a bibliometric analysis for heavy metal removal via micro­
algae (Ubando et al., 2021), The study summarized the application of
various microalgae to remove heavy metals by identifying the different
factors that affect the efficiency of biosorption. More examples are the
use of fish scales (Ighalo and Eletta, 2020), Banana peel (Akpomie and
Conradie, 2020), extremophile microorganisms (Giovanella et al.,
2020), cyanobacterial biomass (Shetty and Krishnakumar, 2020), lig­
nocelluloses (Tran et al., 2019), chitosan (Crini et al., 2019), Tannin
(Santos et al., 2019) and plant leaves (Adeniyi and Ighalo, 2019) as a
biosorbents for the decontamination of water pollutants. It was observed
that most recent review articles have focused on the factors that affect
the biosorption process such as biosorption equilibrium and kinetics in a
typical one biosorbent. The goal of this review is to provide a broader
view of the current research trend, to identify various available bio­
sorbents, to identify potential knowledge gaps, and to explain future
research perspectives.
2. Pollution
2.1. Water pollution
Water is the artery of life on earth. It is one of the main primitive
requirements necessary for livelihood on our planet. It covers more than
71% of the earth’s surface and represents about 70% of its mass. It is the
only substance on the earth naturally existing in three physical states.
The paramount need for pure water cannot be ignored. Regrettably, over
the last decades, the unchecked population expansion and industrial
invasion have led to huge pressure on limited water resources (Calero
et al., 2018). What is worse, innumerable water pollutants are syn­
chronously released into aquatic bodies. It causes severe and accelerated
dramatic deterioration in water quality. Water pollution as a crucial
problem has considerably become a matter of worldwide concern.
Firstly, knowing its nature, main sources, and discredited effects on
human health and the ecosphere is important. Generally, pollution is
environmental contamination, causing acute threats to different biota. It
is mainly classified into five categories including; water, air, soil, bio­
logical and nuclear pollution.
Recently, the overutilization of water resources and water contami­
nation simultaneously occur as a consequence of uncontrolled greed
associated with human civilization. Unfortunately, where people live
and work, wastewater is always found. Several industries are strong
producers of wastewater laden with a great diversity of pollutants. These
pollutants include dyes, heavy metals, phenols, pesticides, insecticides,
and drugs. Discharge of these contaminated effluents into the aquatic
environment has extremely tremendous impacts on our biosphere. It
exhibits immunogenic, teratogenic, mutagenic, and carcinogenic char­
acteristics (Azari et al., 2019). It is well known that about 70–80% of all
illnesses cases in developing countries are related to water pollution
(Qadri and Faiq, 2020).
2.1.1. Sources of water pollution
Two foremost categories that contribute to water pollution can be
classified into two main groups; point and non-point sources.
Point sources: It originates from a single source such as effluent
outfalls from different sewage systems. Other sources are oil wells,
factories, power plants, and refineries. Annually, about 300–400 MT of
different harmful pollutants is directly discharged into water systems.
(ii) Non-point sources: This type of pollution originates from multi­
ple sources. Its release is related to the movement of originated water
from the natural process. According to (NORMAN Network) report,
more than 700 listed environmental contaminants exist in the European
aquatic bodies (Kar et al., 2019). These include heavy metals, dyes,
agrochemicals, oil products, and pharmaceuticals. Additionally, the
European Union reported that other pollutants are found in water bodies
(Barbosa et al., 2016). They include natural hormone (17-b-estradiol
(E2)), synthetic hormone 17-a-ethinylestradiol (EE2)), pesticides
A.M. Elgarahy et al.
(oxadiazon, imidacloprid, methiocarb, thiamethoxam, and triallate),
pain killer diclofenac, major macrolide antibiotics (clarithromycin,
azithromycin, and erythromycin), triallate), UV filter and dyes
additives.
2.2. Petroleum pollution
Natural petroleum production processes are the main sources of
petroleum or crude oil and its derivatives (Jain et al., 2019). It includes
extraction, storage, transportation, ships, marine terminals, and parking
lots. Petroleum accidents related to oil tankers, pipelines, and oil rigs
also participate in water pollution. Approximately, 5 million tons of
petroleum products enter aqueous systems from oil spills (Bo et al.,
2017). Petroleum produced water is known to be one of the most
destructive types of water pollution. It has carcinogenic and mutagenic
features because of its complex nature. It is laden with a mixture of
naphthenic, paraffinic, polycyclic aromatic hydrocarbons (PAHS), trace
amounts of sulfur, oxygen, and nitrogen compounds (Gao et al., 2019).
Accumulation of these persistent compounds in the aquatic environment
negatively impacts the health of different environmental compartments.
2.3. Sewage pollution
Sewage contamination has become a growing global issue resulting
from rapid industrialization. It is largely unrecognized with >50% of the
world’s population census living with coastal cities (Abaya et al.,
2018a). Untreated sewage is introduced into water assets from acci­
dental spills of treatment plant failures. It includes sewer overflow,
broken sewer pipes, clogged lift stations, and effluents discharged from
onsite sewage disposal systems. Environmentally, it represents a com­
plex problem because it contains a cocktail of elevated hazardous levels
of the pollutant. It contains pathogens (bacteria and viruses), inorgani­
c/organic compounds, endocrine disruptors, and hydrocarbons (Ahmed
et al., 2018). It causes detrimental effects on human health as well as
coastal ecosystems. Human exposure to contaminated sewage results in
skin and urinary tract infection, hepatitis, and gastroenteritis. Further­
more, it also negatively influences coral reefs that are considered one of
the most economically valuable and biologically diverse ecosystems on
the earth. Increased coral disease prevalence in addition to severity has
been linked to it (Abaya et al., 2018b).
3. Major pollutants
Owing to different municipal, agricultural, and industrial activities,
numerous industries particularly implicated in water pollution
(Özdemir et al., 2019). Currently, the purification of aqueous effluents
contaminated with toxic chemicals has become a serious environmental
burden (Dallel et al., 2018). Their existence in water bodies beyond
guidelines is unsolicited. They simultaneously provoke serious threats
for both the ecosphere and human health. These pollutants have
non-biodegradable, highly toxic, and carcinogenic characteristics. Even
at low concentrations, it can cause rigorous damage to different
ecosystem compartments (Nguyen et al., 2016). Among the multitude of
pollutants, toxic heavy metals and synthetic organic dyes have been
ecologically causing more worldwide concerns.
3.1. Dyes
Colorants are substances having the capability of transmitting their
color to the other substrates. Mainly, it can be used in a single case or in
combination with other ingredients. They are greatly consumed in
innumerable industries such as plastics, prints, photographs, clothes,
paints, and ceramics. Generally, colorants are divided into two main
classes namely, dyes and pigments (Pavithra et al., 2019). Dyes are
organic compounds, used to impart color to various substrates like
paper. They are capable to bind themself to the external surfaces of
3
Cleaner Engineering and Technology 4 (2021) 100209
different subjects or fabrics. Whereas pigments require another sub­
stance, called a binder, to help them adhere to the substrates (Har
Bhajan and Bharati, 2014). Commercial dyes are broadly categorized in
several ways in terms of the source of origin, chemical structure, color,
and applications as shown in Figure S2 (see supplementary material).
Based on origin, dyes are classified into natural and synthetic dyes.
Natural dyes are derived or extracted from natural resources including
animals, minerals, plants, and invertebrates. Majorly, they are obtained
from vegetable and archeological sources. They are characterized by
numerous merits such as harmonized nature, cost-effective, biodegrad­
ability, and easy disposal. However, the mentioned advantages, the
rampant industrial activities in addition to uncontrolled civilization
growth move people away from natural dyes usage. Because of its dis­
abilities to meet the rapid industrial progress demand, it is mostly
consumed in food industries (Li et al., 2019). Contrarily, synthetic dyes
are fabricated from organic or inorganic compounds and used as alter­
nates to natural dyes. The term synthetic is related to the chemical
structure of the chromophore group. It is primarily made from aniline or
chrome. Each type has a different behavior based upon light fastness and
brightness degree. One exposed to sunlight; aniline (coal tar) dyes fade
easily, while chrome dyes are colorfast and non-corrosive in nature
(Fontana et al., 2018). Dealing with synthetic dyes requires taking into
account numerous critical parameters. They include fading, boiling,
machine washability, dry cleaning, gas fume fading, saltwater, steam
pressing, and perspiration. Also, they can be classified based on their
dissolution behavior in an aqueous medium. Dyes can be divided into
three categories: (a) cationic (basic dyes), (b) anionic (acid, direct, and
reactive dyes), and (c) nonionic (disperse dyes) (Sakin Omer et al.,
2018). Several industries such as carpet and rubber largely used them to
provide different products with attractive colors (Reck et al., 2018). All
these dyes are naturally soluble in water except disperse and vat dyes.
Dyes also contain traces of elements like lead, zinc, copper, chromium
and cobalt. Due to their complex chemical structures, synthetic dyes are
mostly stable against oxidation agents. It leads to increase the chemical
oxygen demand and hence being harmful to aquatic biota and human
health. They adversely affecting on the metabolic processes of micro­
algae as well as aquatic plants. Table 1 shows various classes of dyes
(Kausar et al., 2018), chemical properties and its undesirable effects
(Pavithra et al., 2019).
3.1.1. Chemical properties of some common biosorbed dyes
3.1.1.1. Methylene blue. Methylene blue dye (MB), known as methyl
thioninium chloride, is a heterocyclic aromatic chemical compound
with the molecular formula [C16H18N3SCl]. It is classified as a cationic
dye (Peres et al., 2018). It is consumed in various fields like drugs,
dyestuff industries, paper, textile, and pesticide industries (Elwakeel
et al., 2021b). Some of the undesirable negative effects on human health
are heart palpitations increase, shock, vomiting, jaundice, cyanosis,
quadriplegia, and tissue necrosis (El-Moselhy and Kamal, 2018). A huge
amount of MB (>7.0 mg kg− 1) can lead to high blood pressure, mental
disorder, nausea, and abdominal pain (Lyu et al., 2018).
3.1.1.2. Crystal violet. Crystal violet (CV) (or gentian violet) is a tri­
aminoarylmethane dye with the chemical structure C25H30N3Cl. It is
classified as cationic dyes. It is extensively used in different industries
such as pharmaceutical, paper, textile, and printing ink (Abbasi et al.,
2017) and (Elwakeel, K. Z. et al., 2017). It is harmful, depending on
concentration, by different ways of exposure (inhalation, ingestion, and
skin contact). It is carcinogenic and can cause digestive tract, skin, and
eye irritation in humans (Muthukumaran et al., 2016).
3.1.1.3. Reactive black 5. Reactive black 5 (RB5), C26 H21N5Na4O19S6,
is a type of diazo acidic reactive dyes. It has two sulfonate groups and
two sulfato-ethylsulfon groups in its molecular structure with a negative
A.M. Elgarahy et al. Cleaner Engineering and Technology 4 (2021) 100209

Table 1
Various classes of dyes and their serious health effects.
Dye name Examples Usage method Solubility Nature Applications Health effects References

Direct Direct black, Applied directly to the substrate. Soluble in anionic Cellulose, Cotton, and Bladder cancer carcinogen Kausar et al.
dyes Direct blue. water. blended fibers. (2018)
Reactive Reactive red, The reactive group reacts with fiber Soluble in anionic Cellulosic fiber and Allergic respiratory problem Dawood and
dyes Reactive black polymer. water. fabric. Sen (2014)
5.
Acid dyes Acid red 57, Neutral as well as acidic dye baths Soluble in anion Leather, silk, wool, paper, Burns and skin, mucous Abusaif et al.
Congo red. are used. water. and synthetic fibers. membrane irritation (2021)
Basic dyes Methylene – Soluble in – Cotton, wool, and silk. Carcinogens, allergic skin McYotto et al.
blue, malachite water. reactions, allergic dermatitis, (2021)
green skin Irritation, mutations,
cancer.
Vat dyes Vat Green 6, Fabric is padded in stable dispersion Insoluble in – Blended Fibers, cellulose, Severe burns, skin and Yang et al.
Indigo. often microdispersion to the dye water. and cotton. mucous membrane irritation (2021)
Disperse Disperse blue, Successive treatments with Insoluble in Cation PVC industry, Vilene, DNA damage, induction of Vendemiatti
dyes Disperse solutions of two chemical water. velvets, cellulose acetate, bladder cancer in humans, et al. (2021)
yellow. components that react to form dye nylon, and synthetic splenic sarcomas
on the fibre surface. fibers.
Sulfur – Converted to water-soluble Insoluble in Alkaline Cellulose fiber and – Zheng et al.
dyes substantive form before application. water. cotton. (2021)

charge in aqueous solutions. It characterizes by a simple dyeing pro­
cedure and covalent binding with cellulose fibers (Jóźwiak et al., 2017).
Commonly, it is one of the most reactive dyes used to a large extent of
different fixtures such as cotton. The presence of RB5 in aqueous solu­
tions is of great concern because of its toxic, carcinogenic, and muta­
genic characteristics (Nematollahzadeh et al., 2015). It adversely affects
the biotic communities’ aquatic ecosystem (fauna and flora) and has
direct toxicity to humans. It can cause severe damage to the liver,
digestive, and central nervous systems of human beings (Elwakeel et al.,
2016).
3.1.1.4. Congo red. Congo red (CR) is the sodium salt of 3,3′ -([1,1′ -
biphenyl]-4,4′ -diyl)bis(4-aminonaphtalene-1-sulfonic acid). Its chemi­
cal structure is [C32H22N6Na2O6S2] (Thanh Tu et al., 2018). It is clas­
sified as an anionic dye. Once, it solubilizes in water, it yields a red
colloidal solution. It is used in many fields such as biology, biochemistry,
and the textile industry (Aliabadi and Mahmoodi, 2018). It has many
negative effects on human public health including vomiting, nausea,
diarrhea, allergic problems, and difficulty in breathing. Also, it is easily
metabolized to benzidine, which is identified as having possible carci­
nogenic effects for humans (Deng et al., 2018). Chemical structures of
different mentioned dyes are shown in Figure S3 (see supplementary
material).
3.2. Heavy metals
Surface and groundwater contamination by toxic heavy metals were
globally reported as a serious threat to different water resources. They
are inorganic notorious contaminants with a relatively high atomic
weight between 63.5 and 200.6, and a density greater than 5 g cm− 3.
Different types of heavy metals, anthropogenic sources, toxicity, and
their permissible limits are shown in Table 2 (Kobielska et al., 2018).
They enter the environment through geological and anthropogenic
sources. They are indispensable, relatively poisonous at low concen­
trations, and can be found within the different environmental com­
partments (Alonso-Magdalena et al., 2019). Commonly, heavy metals
are found in rock-forming minerals. Copper, cobalt, manganese, nickel,
zinc, and vanadium are examples of heavy metals that easily leach
because of mineral weathering (Chen et al., 2019). Soil represents
another medium for heavy metals storage. Heavy metals are found in
soils in different forms. Contaminated surface waters can lade heavy
metals over great distances (Richards et al., 2019). Other factors such as
physical, chemical, and biological are considered large contributors to
heavy metals contamination. Whereas, anthropogenic sources are
implicated in groundwater contamination. Groundwater is the main
source of drinking water. It is mainly polluted by both inorganic and
organic contaminants from various anthropogenic sources. This includes
runoff from agricultural sites, sewage systems, motorways, railways,
landfills, urban areas, and so on. Human industrial activities are
considered to be major contributors to environmental pollution by toxic
heavy metals (Ibrahim and Fakhre, 2019). Considerably, several in­
dustrial activities such as coin production and coal combustion generate
a huge amount of heavy metals laden wastewater. It includes arsenic,
cadmium, cobalt, copper, chromium, lead, zinc, iron, manganese,
nickel, mercury, and others. These effluents are dumped into water
systems without proper manipulation (Liu, J. et al., 2019a). Heavy
metals are classified into non-essentials and essential components
necessary to biological and metabolic activities. As, Pb, Cd, and Hg are
categorized as non-essential components to metabolic functions.
Because of their non-biodegradability and bioaccumulation behavior,
they are very toxic even at trace levels (Huang et al., 2019). Therefore,
due to their deleterious nature, they have been ranked in the top 20 list
of dangerous substances as reported by the United States Environmental
Protection Agency (US EPA) and the Agency for Toxic Substances and
Disease Registry (ATSDR). Whilst Cu, Co, Fe, Mn, Zn and Cr(III) are
essential components for human health. They are associated with mul­
tiple metabolic processes of biota including cytochromes and enzymes.
However, excessive exposure to these metals can lead to severe haz­
ardous impacts on different biota. Maximum contamination levels of
different heavy metals are set by World Health Organization (WHO). It
confirms that zero or only the allowable levels should be in water
sources and hence ensure water safety for human usage or consumption.
Severe detrimental effects on ecosystems as well as health hazards are
generated form existence of heavy metals in water systems. Their
presence in water courses can pose major threats to living creatures.
They are very toxic to aquatic ecosystems, adversely affect on plants,
invertebrates, fish and amphibians (Sun et al., 2019). Additionally, they
cause serious health problems on human beings. Various diseases such
as autoimmunity, cancer, developmental retardation, kidney damage
and even death in severe cases are associated with exposure to heavy
metals (Arshad et al., 2019).
Copper(II) as an example of heavy metals is a chemical element
naturally abundant in different compounds. It is the third most wide­
spread metal commonly used by mankind in the industrial sector. Its
annual discharge rate is estimated to be 939,000 metric tons (Blagojev
et al., 2019). It is primarily found in a variety of cells and tissues. It has
many oxidation states but the divalent state Cu(II) is the most toxic
oxidation state. Copper-laden wastewater is originally discharged from
different industrial activities (do Nascimento et al., 2019). Despite its
dangerous nature, it is considered to be an essential micronutrient to

4
A.M. Elgarahy et al. Cleaner Engineering and Technology 4 (2021) 100209

Table 2 Table 2 (continued )

Anthropogenic sources of common heavy metals and metalloid, their toxicity, Heavy Anthropogenic Toxicity Provisional References
and their provisional WHO limits. metal or sources maximum
Heavy Anthropogenic Toxicity Provisional References metalloid tolerable
metal or sources maximum daily intake
metalloid tolerable (PMTDI) (g
daily intake L− 1)
(PMTDI) (g measuring and Minamata
L− 1 ) apparatus, disease.
As Animal feed Phytotoxic (toxic 0.01 Cui et al. catalysts, dental
additive, to plants), (2021) fillings, Hg vapor
algaecides, arsenicosis (i.e. lamps, X-ray
herbicides, Blackfoot tubes,
insecticides, disease), pharmaceuticals,
fungicides, keratosis, fungicides,
pesticides, possible vascular scientific
rodenticides, complications, instruments,
sheep dip, and carcinogenic. electrodes,
tanning and rectifier,
textile, pigments, oscillators, and
veterinary chloralkali cell’s
medicine, mobile cathode.
ceramics, special Ni An alloy in the Contact 0.07 Özdemir
glasses, steel industry, dermatitis, et al.
metallurgy, computer asthma, and (2021)
electronic components, chronic
components, non- catalysts, ceramic respiratory
ferrous smelters, and glass molds, infections
electrical electroplating, carcinogenic.
generation (coal nickel-cadmium
and geothermal), batteries, dental
light filters and and surgical
fireworks. prostheses, arc-
Cd Neutron Phytotoxic, bio- 0.003 Nandi and welding, rods,
absorbers (within accumulative, Chowdhuri and pigments.
nuclear reactors), itai-itai disease, (2021) Zn Zn alloys, PVC Relatively not 0.3–1.0 mg Kobielska
nickel-cadmium and carcinogenic. stabilizers, gold detrimental to kg− 1 of et al.
batteries, anti- precipitation mammals (may body (2018)
corrosive metal from cyanide affect cholesterol weight per
coatings, alloys, solution, in metabolism in day
plastic stabilizers, chemicals and humans).
coal combustion, medicines, anti-
and pigments. corrosion
Cr Data storage, Cr3+ not 0.05 Kobielska coating, cans,
plating, detrimental to et al. barriers, rubber
ferroalloys mammals, Cr6+ (2018) industry.
manufacturing, very toxic and
textiles and carcinogenic.
leather tanning, human health. Its required daily intake value varies between 0.9 and 2.2
wood treatment, mg for adults (Moreira et al., 2019). WHO and US EPA have set the
passivation of threshold limits of 2 (mg L− 1) and 1.3 (mg L− 1) for copper, respectively
corrosion of
cooling circuits,
in drinking water (Safari et al., 2019). Excessive intake of copper is
and pigments. harmful to animals and humans because of its bioaccumulation char­
Cu Water pipes, Relatively not 2 Costa et al. acter. At high concentrations, it can cause harm to the skin, brain,
chemicals and detrimental and (2020) myocardium, liver, pancreas, kidney, and reproductive system (Peng
pharmaceutical narrow tolerance
et al., 2019). Its high existence is also associated with depression, central
equipment, for plants.
kitchenware, nervous system disorders, gastrointestinal irritation, cirrhosis, lung
roofing, alloys, cancer, and even death (Liu et al., 2018).
and pigments.
Pb Alloys, ceramics, Pb poisoning (a 0.01 Cho et al. 4. Biosorption
plastics, world-wide issue) (2020)
glassware, lead- through gasoline,
acid batteries, plumbing, and 4.1. Biosorption fundamental
cable sheathings, paints.
sheets, solder, Biosorption is a practical application branch of sustainable devel­
pipes and tubing,
opment (biotechnological approach) (Işıldar et al., 2019). It is counted
sheets,
ordinance, upon as an eco-friendly, economic, and efficient technique for water
antiknock agent, treatment (Gupta et al., 2018). It minimizes the concentration of
tetramethyllead, different water pollutants to the acceptable limits recommended by
and pigments. different federal regulations (Krstić et al., 2018). This green protocol is
Hg Amalgamation Biomagnification 0.006 Frachini
(the process of in aquatic et al.
in coincidence with the principles of green chemistry. The involved
metal extraction), environments (2020) fundamentals of biosorption process related to its different ingredients
electrical and should be comprehended. Briefly, it is defined as a
metabolism-independent process (passive uptake), built on using of

5
A.M. Elgarahy et al.
bio-wastes for the elimination of different water pollutants. Generally,
numerous benefits are achieved due to the recycling of these biomasses
(bio-wastes). Their utilization in their native and/or modified forms
directly participates in wastes minimization. This can rectify many
ecological and environmental problems (Gupta et al., 2019). It also
characterizes by remarkable merits such as low operating and
manufacturing cost and high efficiency.
4.2. Biosorption strategy
In recent years, biosorption conception as a multidimensional
effective process has been evolving. It is perceived as an alternate
admirable wastewater treatment compared with other traditional tech­
nologies (Demey et al., 2019). Sorption is mainly described as
Physico-chemical phenomenon by which sorbate molecules concentrate
on the surface of another substance (sorbent). This provides purified
effluents with high qualities. Despite denoting a biological entity
involvement by using the “bio” prefix, biosorption term is also simply
defined. Both bioabsorption and biosorption dimensions are involved in
terms of sorption mechanism. Absorption is the incorporation of a
substance in one state into another substance with a different state. It
includes the absorption of gases by water or liquids by a solid). While
adsorption is a physical attachment in which sorbate interacts with a
sorbent resulting in a sorbent-sorbate interface (Fomina and Gadd,
2014). Briefly, biosorption is a passive, metabolically-independent
process covering all interaction aspects between any sorbate and bio­
logical matrix (biosorbent). It plays a crucial part in many processes
naturally occurring in different scientific disciplines.
4.3. Selection of biosorbents
The suitability of biosorbent is known to be the foremost important
step in controlling their selection. Biomass cost and its origin represent a
vital criterion to be considered during biosorbent selection. Dead
biomass has priority over the viable ones to be used for the preparation
of different biosorbents (Elwakeel et al., 2012). Employing of dead
biomass has many merits. It is summarized as (1) absence of the need of
growth requirements (i.e. media, nutrients) to be contained in the feed
solution; (2) absence of toxicity limitations; (3) possible reusability and
recovery of saturated biosorbent and sorbed pollutants, respectively; (4)
easier mathematical and statistical modeling of pollutants uptake.
Additionally, the selected biosorbent should have numerous requisite
aspects such as eco-friendly, availability, biocompatibility, and feasi­
bility. This ensures its potential capacity to detoxify different water
pollutants. Other diversified admirable features characterized by bio­
sorbent are required. This includes its high sorptive performance to­
wards target pollutants, good stability, and its reusability. Recyclability
and adaptability of biosorbent to different designs (i.e. batch, fixed bed
systems) should significantly be considered (Elwakeel, 2010). Based on
wastes as wealth, utmost attention should be given to the available
wastes. Their utilization offers multiple benefits because of their envi­
ronmentally benign nature. It is economically beneficial because it
overcomes disposal problems and generates revenue for different in­
dustries. In reality, the plentiful biological materials are substantially
different in structure. They consist of a variety of ligands like alcohol,
amino, aldehydes, carboxylic, hydroxyl, phosphate, thiol, ketones,
phenolic, and ether groups. They are present at varying degrees and
hence being capable to interact with target pollutants via different
mechanisms.
Biosorption represents a promising and alternative to conventional
processes. It depends on using bio-wastes for different water polluter’s
removal. Its theory is built to make a double benefit from these bio-
wastes. This is done by recycling it to directly participate in wastes
minimization in addition to extract maximum benefits from it (Gupta
et al., 2019). Consequently, it allows reaching the abatement levels
endorsed by international or national regulations and WHO (Hespanhol
6
Cleaner Engineering and Technology 4 (2021) 100209
and Prost, 1994) It characterizes by remarkable merits such as low
operating and manufacturing cost, flexibility, ease of operation, and
high efficiency. Various biosorbents based on: (i) chitosan (Almughamisi
et al., 2020); (ii) biochar (Lei et al., 2019); (iii) activated carbon
(Elwakeel et al., 2015); (iv) bio-nanocomposites (Jung et al., 2019); (v)
bio-hydrogels (Qi et al., 2019); (vi) macroalgae (Elgarahy, Ahmed M.
et al., 2019); (vii) agriculture wastes (Toumi et al., 2018); and (vii)
bio-calcium carbonate (Arslanoğlu, 2021) were used for water refine­
ment from different pollutants including toxic dyes and heavy metals.
Marine algae are considered as alternative and effective based sor­
bents for the manipulation of wastewater. It considers renewable re­
sources spread all over the world. It can be categorized based on its color
and colloid content. Generally, three basic groups are normally found in
oceans: Chlorophyta, Phaeophyta, and Rhodophyta algae (Mokhtar
et al., 2017). The use of microalgae as a sustainable alternative has been
demonstrated in recent studies. Afshariani and Schneider (Afshariani
and Roosta, 2019), for example, studied the sorption of methylene blue
by batch and continuous processes in aqueous solutions. At pH 9 and a
temperature of 30 ◦ C, the maximum sorption reached 87.69 ± 3.22 mg
g− 1. The use of defatted microalgae biomass (microalgae biofuel waste)
as an alternative leather dye adsorbent was examined (da Fontoura
et al., 2017). Biosorption experiments were carried out with Acid Blue
161 aqueous dye solutions (AB-161). A dye was adsorbed with a
maximum amount of 75.78 mg g− 1 and 83.2 mg− 1 at 25 ◦ C and 40 ◦ C,
respectively. The findings showed that biomass decreased dye concen­
trations substantially 76.65% from true tannery wastes effluents. Poly­
saccharides are the main components of the algal cell wall which
consists of alginate, carrageenan, and polycolloid. These constituents
have the capabilities for the removal of different water pollutants
(Daneshvar et al., 2017). Both macro and microalgae were utilized as
excellent candidates for different organic dyes (da Rosa et al., 2018); as
well as heavy metals elimination from aquatic systems (Chen et al.,
2019). The ability of green macroalga (Enteromorpha flexuosa) to capture
both crystal violet (CV) and methylene blue (MB) from aqueous solu­
tions was evaluated (Elgarahy, Ahmed M. et al., 2019). The results
showed that percentage removal of 90.3% and 93.4% were obtained
under optimum conditions of variables for CV and MB, respectively
(Elgarahy, Ahmed M. et al., 2019). Green algae mainly consist of cel­
lulose associated with a high percentage of proteins combined with
polysaccharides to form glycoproteins (Jayakumar et al., 2014). These
compounds characterize by possessing numerous functional groups (i.e.
amino, hydroxyl, and carboxyl). They play a prominent role in the
sorption process (Rangabhashiyam et al., 2016).
Brown algae characterize by possessing a broad range of metabolites
such as alginates, fucoidans, mannitol, laminarins, fucoxanthin, halo­
genated compounds, polyphenols, and terpenoids (Saravana et al.,
2018). Alginates are a mixture of calcium, phosphate, and sodium salts.
Sodium salts are the major constituents naturally present in the brown
seaweed cell wall. It is nearly up to 30–40% in its weight. It is linear
anionic and water-soluble polysaccharides (Fernando et al., 2019).
Different pre-extraction treatment methods were used for obtaining
alginate from brown seaweed (Saravana et al., 2018). There is a great
use of these natural biopolymers in different environmental applications
(Cardoso et al., 2017). Referring to possessing different functional
groups, it is widely used as a potential sorbent for treating wastewater
from various water pollutants (Elgarahy et al., 2021).
Biochar derived from microalgae pyrolysis as another type of sor­
bents for heavy metals removal from aqueous solution was investigated
by several researchers (Amin and Chetpattananondh, 2019). Many ex­
periments on the efficiency of the Co(II) removal biochar have been
performed in a batch system. The equilibrium data were well fitted for
Freundlich, Temkin, and D-R isotherms. The Langmuir biosorption ca­
pacity reached 1.117 mg g− 1 (Bordoloi et al., 2017). Biochar produced
from water hyacinths (Eichhornia crassipes) was demonstrated to be an
effective sorbent for the removal of certain heavy metals and as a means
of control for this highly invasive species. Harvesting water hyacinth
A.M. Elgarahy et al.
biomass as feedstock for biochar has the additional advantage of
reducing its impact as an invasives species on sensitive aquatic habitats.
biochar-alginate capsules were examined to remove Cd(II) from an
aqueous solution with the maximum sorption capacities ranging from
24.2 to 45.8 mg g− 1 (Liu et al., 2020).
Recently alginate and sericin particles chemically crosslinked with
poly(vinyl alcohol) (SAPVA) for batch biosorption of rare-earth element
ytterbium from the aqueous medium was investigated (da Costa et al.,
2020), The equilibrium study showed that the maximum biosorption
capacity for ytterbium was 0.642 mmol g− 1 at 55 ◦ C (da Costa et al.,
2020). To increase the sorption properties of alginate gel beads, sodium
alginate-based beads with different amount of pore-forming agent were
prepared with calcium carbonate as the pore-forming agent (Hu, X.
et al., 2020). The experimental results showed that the adsorption ca­
pacity of Cu(II) increased by at least two times (from 13.69 mg g− 1 to
33.88 mg g− 1) (Hu, X. et al., 2020). Another recent way for alginate
modification was carried out, alginate-PEI beads were functionalized by
phosphorylation and applied for the sorption of Nd(III) and Mo(VI) (Wei
et al., 2020). The sorption of Nd(III) is strongly increased by phos­
phorylation, while for Mo(VI) the enhancement is rather limited by
phosphorus groups. The phosphorylation of alginate-PEI beads
increased Nd(III) maximum sorption capacity from 0.61 to 1.46 mmol
g− 1, The enhancement of Mo(VI) uptake is much less marked (from 1.46
to 2.09 mmol g− 1) because of the high affinity of molybdate species for
amine groups (Wei et al., 2020).
Chitosan is a derivative of chitin. It is made predominantly from
shellfish waste items like crab or shrimp shells (Elwakeel, 2010). The
comparison of the sorption properties of 6 different crosslinking agents
crosslinking chitosan sorbents (3 ionic agents: sodium citrate, sodium
tripolyphosphate, sulfosuccinic acid, and 3 covalent agents: glutaral­
dehyde, epichlorohydrin, trimethylo propane, triglycidyl ether) was
examined. (Jóźwiak and Filipkowska, 2020). Ionic crosslinking signifi­
cantly affected the sorption capacity of the chitosan hydrogel towards
Reactive Black 5 dye (Jóźwiak and Filipkowska, 2020). The sorption
potential of 46.7% and 37.2% for chitosan crosslinked with sodium
citrate and sulfosuccinate was higher compared to non-crosslinked
chitosan after 24 h of the sorption process (Jóźwiak and Filipkowska,
2020). Conversely, chitosan crosslinked with glutaraldehyde and tri­
methylopropane triglycidyl ether showed to have a 35.3% and 26.6%
lower sorption potential after 24 h of sorption than that of unmodified
chitosan. Once the sorption equilibrium had been reached, the highest
sorption capacity (2307 mg g− 1) was displayed by the unmodified chi­
tosan, whereas sorption capacities of the ionically crosslinked hydrogels
were in the range of 2005–2164 mg g− 1 and these of the covalently
crosslinked hydrogels were in the range of 2083–2183 mg g− 1 (Jóźwiak
and Filipkowska, 2020). To remove cationic crystal violet (CV) and
anionic methyl orange dye (MO) from wastewater, polypyrrole deco­
rated chitosan-based mag-sorbent was prepared. Removal performance
was obtained to be 88.11 and 92.89% for CV and MO at the optimum
conditions. The pseudo-second-order represented the adsorption of CV
well, while the pseudo-first-order kinetics better followed that of MO.
Langmuir adsorption isotherm with a maximum monolayer sorption
potential of 62.89 and 89.29 mg g− 1 for CV and MO, respectively, was
well matched to the adsorption equilibrium data for both dyes. Another
way for chitosan modification is to be immobilized on another polymer.
For example, chitosan was successfully modified with 4-methyl-2-(naph­
thalen-2-yl)-N-propylpentanamide-functionalized ethoxy-silica (Jabli,
2020) then tested for methylene blue (MB) and Acid blue 25 (AB25).
Using composite beads, the adsorbed yield of MB increased three times
more than the capacity of chitosan beads, and in the case of AB25, it
improved 1.4 times. Another chitosan hybrid composite was prepared
by doping a very small amount of chitosan and Y(III) ions onto the
acid-modified fly ash (named as MFA) the saturated adsorption capacity
reached up to 627 mg g− 1 (Li and Ren, 2020). A lot of effort was done by
the researchers to increase the selectivity of chitosan towards specific
metal ions. For example, the grafting of 2-mercaptobenzimidazole onto
7
Cleaner Engineering and Technology 4 (2021) 100209
chitosan microparticles allows developing highly selective sorbents. The
incorporation of magnetite particles is also a strategic aspect for facili­
tating the use and recovery of chitosan microparticles (Elwakeel et al.,
2021a). The sorbent showed high selectivity for precious metals against
base metals. The combination of chitosan and 2-MBI allows designing a
very efficient sorbent for the recovery of precious metals from acidic
leachates (Elwakeel et al., 2021a). The adsorption capacities of the
heavy metal ions (manganese, iron, cobalt, nickel, copper, and zinc) on
chitosan were investigated in dependence on their corresponding anions
sulfate, chloride, and nitrate by batch experiments (Weiβpflog et al.,
2020). The selectivity of the different heavy metal ions was analyzed by
column experiments. The heavy metal cations of the sulfate salts and the
sulfate ions themselves adsorb to a significantly higher extent compared
to the analogous chloride and nitrate salts, respectively (Weiβpflog
et al., 2020). Luo et al. (2020) prepared fluorescent chitosan-based
hydrogel incorporating titanate and cellulose nanofibers modified
with carbon dots to effectively remove Cr(VI) (Luo et al., 2020). The
sorbent had a higher adsorption ability of Cr(VI) (maximum adsorption
capacity, 228.2 mg g− 1), maybe mainly attributed to the porous struc­
tures and the additional titanate and cellulose nanofibers modified with
carbon dots improving the sorption ability of Cr(VI) (Luo et al., 2020). A
series of magnetically modified chitosan sorbents with core-brush to­
pology were prepared through grafting co-polymerization on the surface
of chitosan/Fe3O4 composite particles, and then applied for the removal
of two pharmaceuticals (diclofenac sodium) and tetracycline hydro­
chloride) from water (Zhang et al., 2016). This study provided a strategy
for the design of adsorbents from both topological and chemical struc­
tures (Zhang et al., 2016). All the modified chitosan sorbents exhibited
higher removal efficiencies, due to the enhanced surface areas and
functionalization (Elwakeel et al., 2014).
A series of novel chitosan/nanodiamond (chitosan/ND) composites
containing NDs with variable surface carboxyl groups and various
concentrations were prepared using the solution casting method. Pow­
dery chitosan/ND composites were employed as the adsorbent of a
model anionic dye (methyl orange, MO). Experimental results showed
that the incorporation of NDs with high carboxylic content (ND-H) into
chitosan increased substantially the maximum adsorption capacity of
neat CTS from 167 mg g− 1 to 454 mg g− 1. The remarkable adsorption
capacity of dye on chitosan/ND composites was associated with the
oxygen-containing groups on the outer surface of NDs which would be
beneficial to interact with the dye molecules through hydrogen bonding
and electrostatic interactions (Raeiszadeh et al., 2018).
Calcium carbonate (CaCO3) is considered one of the most versatile
materials known to man. It is widespread and represents above four
percent of the total earth’s crust. CaCO3 is found in many common forms
as chalk, marble, and limestone. Bio-calcium is mainly produced from
shells of aquatic biota such as bivalves, corals, and snails (Elwakeel
et al., 2020). It carbonate can be found in three main forms: aragonite,
calcite, and vaterite (Hoque et al., 2013). Though all these forms are the
same chemically, it varies in other physical aspects as whiteness, ho­
mogeneity, thickness, and purity. Due to its special white color, CaCO3 is
extensively used in the cement industry. It has also wide applications as
a filler and/or coating pigment in coatings facilities as well as plastics,
paints, and paper industries (Thilagan et al., 2015). Moreover, CaCO3 is
used in industrial settings to neutralize acidic conditions in both soil and
water due to its antacid properties (Granados-Correa et al., 2013).
Granados-Correa et al. mentioned that CaCO3 benefits the environment
through water and wastewater treatment (Granados-Correa et al.,
2013). It is widely used in the tissue bioengineering field (Dharmaraj
et al., 2015).
Two marine wastes, including sepia shells and bivalve shells, are rich
in CaCO3. Shells of the mentioned aquatic biota act as exterior and
interior skeletons for protecting the soft parts of the molluscan bodies.
Sepia shells (SS) are sub-products of fisheries. They offer mechanical
support against predators. Despite being rich in calcium, they are usu­
ally disposed of without any commercial valorization. This may cause
A.M. Elgarahy et al.
locally some environmental nuisances especially in Port-Said City,
Egypt. The exploitation of this by-product for application in dye removal
would make a double benefit. A literature survey showed that very few
works were performed on dye removal using cuttlefish bones (Hasmath
Farzana and Meenakshi, 2014). Bivalve shells of Anadara uropigimelana
were firstly tested as a potential biosorbent for MB recovery from an
aqueous solution (Elwakeel, Khalid Z. et al., 2017), Percentage removal
of 93.6% were obtained under optimum conditions of variables (initial
pH of 10.4, sorbent dose of 1 g L− 1, initial MB concentration of 20 mg
L− 1, and temperature of 25 ± 1 ◦ C) (Elwakeel, Khalid Z. et al., 2017). On
the other hand, bivalve shells are composed of 95% CaCO3 in addition to
5% of proteins and polysaccharides (Kanyal and Bhatt, 2015). Due to its
structural and superficial properties, it is used as an adsorbent material
for the removal of different pollutants from the environment (Chavan
and Mane, 2013). Calcium chloride (CaCl2) is one of the calcium car­
bonate derivatives that can be directly prepared by reacting to CaCO3
with a hydrochloric solution. Discarded oyster shells were used to pre­
pare vaterite calcium carbonate microparticles and explored the
removal effects and the underlying mechanism toward several heavy
metal ions (Elwakeel et al., 2020). The experimental results showed that
CaCO3 exhibited different removal efficiencies for Pb(II) (99.9%), Cr(III)
(99.5%), Fe(III) (99.3%), and Cu(II) (57.1%) (Lin et al., 2020). Efficient
sorbent based on Sepia shells (cuttlefish bones) was prepared and
examined for the sorption of cationic dye (crystal violet, CV) and an
anionic dye (congo red, CR). The sorbent was modified by the reaction of
sepia shell powder with urea in the presence of formaldehyde (SSBC).
Maximum sorption capacities reach up to 0.536 mmol g− 1 for CV and
0.359 mmol g− 1 for CR, at pH 10.6 and 2.4, respectively (Elwakeel et al.,
2020). Using SSBC Maximum sorption capacities reach up to 0.794
mmol g− 1 (254.05 mg g− 1) for MB and 0.271 mmol g− 1 (269.18 mg g− 1)
for RB5, at pH 10.5 and 2.3, respectively (Elgarahy, A. M. et al., 2019).
Recently, an eco-friendly sorbent based on marine brown algae and
bivalve shells for subsequent uptake of congo red dye and copper(II) ions
was investigated, the maximum sorption capacity reached up to 441 mg
g− 1 (Elgarahy et al., 2020).
Analyzing the reviewed biosorbents, chitosan and alginate-based
biosorbents showed the best sorption capacities for metal ions
removal. Chitosan-based sorbents were the most effective sorbents for
cationic dyes removal, while alginate-based sorbents were the most
effective sorbents for anionic dyes. Alginate was demonstrated to be
more chemically stable. However, the addition of cross-linking agents to
chitosan composites could overcome such a disadvantage.
Generally, numerous benefits will achieve due to the recycling of
these biomasses. Its utilization will participate in wastes elimination.
Additionally, it will minimize contaminant concentrations in different
water resources. This can rectify many environmental problems. Other
remarkable merits such as low operating and manufacturing cost in
addition to high efficiency may be achieved.
4.4. Biosorption capacity and mechanism
Biosorption mechanistic studies of different water pollutants are
critical for appraising their manipulation efficiency. They are beneficial
for optimizing the removal process conditions. Up to now, numerous
studies have focused on investigating possible biosorption interaction
mechanisms. High biosorption efficiency should be characterized by the
biosorbent for the effective elimination of different water pollutants.
Generally, the biosorption process is based on the physicochemical
features of biosorbent. They include solubility, molecular size, surface
charge, chemical composition, reactivity, and hydrophobicity. Gener­
ally, the presence of numerous functional groups facilities the sorption
process of both metal ions and dyes. Commonly, the proposed mecha­
nisms include aggregation, complexation/coordination, electrostatic
interaction, ion exchange, microprecipitation, oxidation, and reduction.
Da Fontoura et al. for example, demonstrated by the thermodynamic
adsorption studies of AB-161 on the micro-algal biomass that the main
8
Cleaner Engineering and Technology 4 (2021) 100209
mechanism is an electrostatic interaction with a spontaneous endo­
thermal process (da Fontoura et al., 2017). However, lin et al., discov­
ered that the heavy metal removal mechanism on calcium carbonate
obtained from discarded oyster shells involves an ion-exchange reaction
between calcium and the heavy metal ions resulting in recrystallization,
which further affected removal efficiency (Lin et al., 2020). The bio­
sorption of strontium and cesium ions onto a marine brown alga
(Undaria pinnatifida) was studied using isothermal titration calorimetry
and molecular dynamics simulation (Hu, Yao et al., 2020b). The main
active sites for metal ion adsorption were carboxyl, sulfate, amine, and
amide. The results confirmed that the chemical sorption was not the sole
sorption mechanism (Hu, Yao et al., 2020b). Fig. 1 shows the different
mechanisms involved in the biosorption process. The possibility of
precipitation as well as crystallization occurrence cannot be ignored.
This simultaneously complicates with sorption and/or desorption pro­
cess. To explore the main biosorption mechanism, variable character­
ization strategies, and theoretical models have been performed. The
interaction between water pollutants and biosorbents mainly occurs in
two different scenarios; surface sorption and interstitial sorption. During
surface sorption, sorbate molecules migrate from the aqueous solution to
the biosorbent surface. Once, pollutants (molecules and/or ions) have
passed through the boundary layer surrounding to biosorbent, they
attach to the active sites found on its surface and subsequently removed
from aqueous solutions. Usually, this type of sorption is achieved by
dipole interactions, hydrogen bonding, or Van Der Waals forces (Suly­
man et al., 2017). Whereas, during interstitial sorption, pollutants
(molecules and/or ions) diffuse towards biosrbent pores (macro, meso,
and/or micropores). Finally, they are biosorbed to the interior surface of
biosorbent (Joseph et al., 2019). Additionally, electrostatic interactions
can explain the tackling of different pollutants from water and waste­
water. They were identified as a major contributor to the biosorption of
water contaminants. The existence of abundant functional groups on the
biosorbent surface makes them typical candidates to efficiently capture
pollutants from different water systems. The capability of these func­
tional groups is significantly influenced by the pH of the medium. Lower
pH values lead to protonation of various functional groups. This leads to
developing a positive charge on the biosorbent surface. Consequently,
electrostatic repulsion occurs, reducing and/or preventing the sorption
of positively charged pollutants. Conversely, electrostatic repulsion de­
clines with raising the medium pH. This leads to an increase in their
biosorption in terms of electrostatic attraction phenomena.
The dissociation constant values (pKa) of biosorbent functional
groups and its (pHPZC) value are relative to pH of the solution. This
influenced the biosorbent sorption capacity. (pKa) values of numerous
functional groups such as carboxylic and phenol groups range from
(3.5–5.5). This indicates that the majority of these groups deprotonate in
this pH working range. So, an enhancement of negatively charged
sorption sites will be available for the biosorption process (Al-Wakeel
et al., 2015). Additionally, the biosorbent (pHPZC) value greatly affects
on biosorption process. The surface charge of the biosorbent is positive
when the pH of the solution < pHPZC. Whereas, its surface charge is
negative when the pH of a solution > pHPZC. As a result, the elimination
of positively charged pollutants is particularly low when pH is lower
than pHPZC. It increases when pH is greater than pHPZC. This approved a
significant involvement of electrostatic forces during the biosorption
process (Ghazali et al., 2018).
The biosorption process can also be interpreted based on the ion
exchange mechanism between the sorbent and the studied pollutants. Its
contribution is explained through the replacement (exchange) of pro­
tons from the exchangeable sites present on biosorbent surface with
pollutants (i.e. metal ions). The mechanism is facilitated by the existence
of hydroxyl, carboxyl, and phenols groups. They can be attached by
pollutant ions via two pairs of electrons and subsequently release two H+
and/or Na+ into the solution (Moreira et al., 2019). The solution pH
influencing the ion exchange mechanism. In the acidic medium, an in­
crease in the H+ ions lead to competition with positively charged
A.M. Elgarahy et al.
Fig. 1. Mechanisms involved in the biosorption process.
pollutants to be sorbed onto the biosorbent. While, in the basic medium,
an increase in the OH− ions leads to competing with negatively charged
pollutants to be sorbed on the sorption sites.
Formation of surface complexes involves the interaction of pollutants
(i.e. metal ions) with oxygen donor atoms from the oxygen-containing
functional groups (coordination). This is associated with the release of
protons and the formation of surface complexes. Ligand tendency for
metal complexes formation is significantly dependent on the metals
classification. Considering, their chemical characteristics, they are
classified based on the hard-soft-acid-base principle. Metal ions (cat­
ions) can bind with biosorbent surface through an inner-sphere or outer-
sphere complex mechanisms. This is carried out through a covalent bond
established between the metal and the oxygen atom (electron donor). It
can also be carried out by cations approaching the negative groups
present on the surface (critical distance). This is associated with the
presence of at least a water molecule between the cation and base,
respectively (Fomina and Gadd, 2014).
Several composite materials based biosorbents were investigated in
the literature, This binary combination between different biosorbents
and different chemical reagents has advantages in the sense of
increasing sorption capacity, enhancement of sorption kinetics, and
renewability. For example, MIL-101(Cr)/sodium alginate (MIL-101(Cr)/
SA) and MIL-101(Cr)/chitosan (MIL-101(Cr)/CS) composite beads were
prepared (Zhuo et al., 2017). Adsorption of three selected pharmaceu­
ticals and personal care products (PPCPs) (benzoic acid (BEN),
ibuprofen (IBU), and ketoprofen (KET)) onto the two composite beads
was investigated and compared with pristine SA and CS beads. Kinetic
plots, pH dependence, isotherm data, and influences of ionic strength
were reported. The MIL-101(Cr)/CS beads exhibit much higher
adsorption capacity than SA, CS, and MIL-101(Cr)/SA, and the adsorp­
tion amounts of three PPCPs onto MIL-101(Cr)/CS follow the order of
KET > IBU > BEN. The adsorption amounts of the three PPCPs on the
MIL-101(Cr)/CS increased quickly during the first 60 min of contact
time and then achieved the adsorption equilibrium after ~180min. Not
only the protonated amine groups but also the Cr center of the adsor­
bents exerted electrostatic attraction with the deprotonated carboxyl
groups of contaminants, as elucidated by X-ray photoelectron spec­
troscopy (XPS). Based on the adsorption isotherms and π-energy analysis
9
Cleaner Engineering and Technology 4 (2021) 100209
of three PPCPs, π-π interaction of aromatic groups between adsorbents
and contaminants also contributed to the adsorption. The MIL-101
(Cr)/CS beads exhibited good renewability over several repeated
adsorption/desorption cycles (Zhuo et al., 2017). Comparison of sorp­
tion capacity and sorption mechanism of different biosorbents are re­
ported in Table 3.
Table 4 summarizes biosorption properties for a series of alternative
biosorbents. Some sorbents have outstanding biosorption capacities and
removal %. The strict comparison of sorption performances is difficult
because of the influence of different biosorption conditions. However,
the reported biosorbents demonstrate very attractive removal percents
due to the high biosorption capacities.
4.5. Future perspectives
A few aspects must be studied to improve the characteristics of the
biosorbents, especially regarding textural properties. There are also
many methods of improvement that have changed the sorption activity
of the biosorbents, such as sonication, freeze-drying, and the incorpo­
ration of other functional groups. Chitosan and alginate have been
extensively investigated in the synthesis of composite beads and films
applied to remove several heavy metals and dyes. Although less studied,
pharmaceuticals and other organic and inorganic contaminants were
effectively sorbed by such materials, indicating a perspective for further
research. Synergistic effects were detected in the reviewed biosorbents,
proving the role of the interaction between different pollutants in the
aqueous medium. This effect was advantageous in the sense of
increasing sorption capacity, enhancement of sorption kinetics, and
renewability. The future direction of research should concentrate on
increasing the biosorption ability of different biosorbents to extract
heavy metals and dyes from industrial wastewater. There has been very
little research on the sustainability evaluation of the removal of heavy
metals by biosorbents in terms of risk, environment, and human health
evaluation. To be competitive with conventional ion exchange resins,
the physical properties of the sorbents need to be improved. It should be
cost-effective, have good mechanical strength, reasonable strength,
durability, and porosity. To fulfill these conditions, several methods
might be used, including grafting onto plastic polymers, binding in
A.M. Elgarahy et al. Cleaner Engineering and Technology 4 (2021) 100209

Table 3
Comparison of sorption capacity and sorption mechanism of different biosorbents.
Biosorbent Water Pollutant Biosorption capacity Biosorption mechanism References
(mg g− 1)

Brown seaweed Sargassum muticum Sb(III) 4±1 Complexation and hydrogen bonding Ungureanu et al. (2017)
Magnetized C. micaceus Hg (II) 26.2 Complexation Özdemir et al. (2019)
Sargassum glaucescens As(III) 116.6 Electrostatic interaction Tabaraki and
Heidarizadi (2018)
Phanerochaete chrysosporium Ni(II) 46.50 Chemical interaction Noormohamadi et al.
(2019)
Renewable durian peels Zn (II) 36.73 Electrostatic interaction Ngabura et al. (2018)
Sulfur functionalized marine brown algae La(III) 185.44 Internal and external diffusion mechanisms Keshtkar et al. (2019)
Cystoseira indica
Gliricidia sepium leaf powder Cr(VI) 35.71 Chelation, Ion exchange, Complexation, Physical (E et al., 2019)
adsorption, and chemical adsorption
Magnetized C. micaceus Co(II) 24.7 Complexation Özdemir et al. (2019)
Yeast Saccharomyces cerevisiae Cu (II) 4.73 Ion exchange Nascimento et al. (2019)
Sargassum glaucescens As(V) 207.3 Electrostatic interaction Tabaraki and
Heidarizadi (2018)
Formaldehyde modified green tomato husk Fe (III) 19.83 Precipitation and ion exchange García-Mendieta et al.
(2012)
bacterium Bacillus amyloliquefaciens U(VI) 179.5 Chemical interaction (Liu, Liu et al., 2019b)
Phanerochaete chrysosporium Cd(II) 71.43 Chemical interaction Noormohamadi et al.
(2019)
Sulfur functionalized marine brown algae Ce(III) 172.33 Internal and external diffusion mechanisms Keshtkar et al. (2019)
Cystoseira indica
Ion-imprinted Tetraethylenepentamine Pb (II) 259.68 Complexation Liu et al. (2016)
modified chitosan beads
Chitin Au 35 Complexation Côrtes et al. (2015)
Formaldehyde modified green tomato husk Mn (II) 15.22 Ion exchange and complexation García-Mendieta et al.
(2012)
Urea calcium alginate beads functionalized with Cu(II) 441 Electrostatic interaction, ion exchange, and Elgarahy et al. (2020)
Congo red dye complexation
Green microalgae Chlorella pyrenoidosa Rhodamine B dye 63.14 Electrostatic interaction da Rosa et al. (2018)
Sepia shells based composite Methylene blue dye 254.05 Electrostatic interaction (Elgarahy, A. M. et al.,
2019)
Sepia shells based composite Reactive black 5 dye 269.18 Electrostatic interaction (Elgarahy, A. M. et al.,
2019)
Magnetic chitosan Glutaraldehyde composite Crystal violet dye 105.467 Electrostatic interaction Azari et al. (2019)
IL modified AC (ILAC) Reactive blue dye 364.4 Electrostatic interaction Lawal et al. (2017)
Ethylenediamine modified fiber btained from Acid Blue 25 dye 67 Van Der Waals’ forces, π-π stacking, and hydrogen Tka et al. (2018)
natural Populus tremula bond
Carica papaya wood Malachite green dye 52.63 Electrostatic interaction (S et al., 2018)
Grape pomace KROM KGT dye 180.2 ± 3.2 Electrostatic interaction Oliveira et al. (2018)
Chemically modified masau stones Orange (II) dye 136.8 Hydrogen bonding and electrostatic attraction Albadarin et al. (2017)
Millimeter-sized chitosan/carboxymethyl Methylene blue dye 64.6 Electrostatic attraction, complexation, hydrogen Kong et al. (2020)
cellulose hollow capsule bond, and van der Waals interaction
Millimeter-sized chitosan/carboxymethyl Methyl orange dye 334.8 Electrostatic attraction, complexation, hydrogen Kong et al. (2020)
cellulose hollow capsule bond, and van der Waals interaction
Millimeter-sized chitosan/carboxymethyl Acid blue-113 dye 526.8 Electrostatic attraction, complexation, hydrogen Kong et al. (2020)
cellulose hollow capsule bond, and van der Waals interaction
Bio sourced composite (activated carbon/TiO2) Diclofenac 153.8 Adsorption, photolysis, and photoinduced El Mouchtari et al.
degradation (2020)
Bio sourced composite (activated carbon/TiO2) Carbamazepine 105.3 Adsorption, photolysis, and photoinduced El Mouchtari et al.
degradation (2020)
Bio sourced composite (activated carbon/TiO2) Sulfamethoxazole 125.0 Adsorption, photolysis, and photoinduced El Mouchtari et al.
degradation (2020)
Biopolymer electrospun nanofibres Carbamazepine 31.25 Chemisorption Kebede et al. (2019)
Biopolymer electrospun nanofibres Ketoprofen 111.11 Chemisorption Kebede et al. (2019)
Biopolymer electrospun nanofibres Fenoprofen 333.33 Chemisorption Kebede et al. (2019)
Biopolymer electrospun nanofibres Diclofenac 125 Chemisorption Kebede et al. (2019)
Biopolymer electrospun nanofibres Ibuprofen 125 Chemisorption Kebede et al. (2019)
Residual defatted biomass (RDB) of the fungus Procion red H–E7B 188.79 Electrostatic interaction Tonato et al. (2019)
Nigrospora sp. dye
Clay Phenol 15.11 Electrostatic interaction Dehmani et al. (2020)
Pine fruit shells PFS (BC550) Phenol 26.738 Dispersive interaction and π-π interaction Mohammed et al. (2018)
Tithonia diversifolia activated carbon Phenol 50.552 Dispersive interaction and π Supong et al. (2020)
Tithonia diversifolia activated carbon 2,4-dinitrophenol 42.607 Dispersive interaction and π Supong et al. (2020)
Biochar derived from corn straw Atrazine 11.566 Electrostatic interaction Zhao et al. (2013)
Corn cob-derived porous carbons (PCs) Phenanthrene 692.27 Pore filling, hydrophobic effects, and π-π stacking Cheng et al. (2019)
interactions

inorganic or organic materials, and cross-linking.
5. Conclusion
This article comprehensively reviewed the biosorption of heavy
metals and organic dyes pollutants using different biomaterials. Bio­
sorbents are an efficient and green approach for dyes and heavy metal
removal from wastewater. A wide variety of physical and chemical
treatments can be applied to modify biomass porosity and surface areas,
thus increasing the number of available sorption sites and binding

10
A.M. Elgarahy et al. Cleaner Engineering and Technology 4 (2021) 100209

Table 4
Comparison of sorption capacity and removal (%) of different biosorbents.
Water Biosorbent pH Biosorbent Temperature Water Pollutant Contact Removal Maximum References
Pollutant dosage (g concentration time percentage uptake
L− 1 ) (mg L− 1) (min) (%) capacity (mg
g− 1)

Methylene Activated Carbon Prepared from 11 0.6 25 ◦ C 100 – 98% 231.48 Üner et al. (2016)
Blue Dye Citrullus lanatus Rind
Methylene Watermelon (Citrullus lanatus) 5.6 0.6 30 ◦ C 50–400 – 85% 188.68 Jawad et al.
Blue Dye rinds (2018)
Congo red Titanium oxide (TiO2) 4.3 0.8 25 ◦ C 14.7 – 101.45% 17 Masoudian et al.
Dye nanoparticles loaded onto (2019)
activated carbon prepared from
bio-waste watermelon rind
Phenol red Titanium oxide (TiO2) 4.3 0.8 25 ◦ C 45.9 – 100% 55.6 Masoudian et al.
Dye nanoparticles loaded onto (2019)
activated carbon prepared from
bio-waste watermelon rind
Basic Brown Durian (Duriozibethinusmurray) 8 1.0 – 15 30 74.26%– – Gopalakrishnan
16 Dye Shell 77.61% et al. (2020)
Orange G Watermelon shell (Citrullus 2 25 30 ◦ C 250 – 100% 27 Chigbundu and
Dye vulgaris) Adebowale
(2017)
Basic red 2 Watermelon shell (Citrullus 4 25 30 ◦ C 250 – 100% 125 Chigbundu and
Dye vulgaris) Adebowale
(2017)
Remazol Aspergillus iizukae 605EAN 6 – – 571.5 12,312 78.34%– – Noman et al.
Brilliant (8.55 80.00% (2020b)
Blue R days)
Dye
Crystal Pectin 2 0.25 – 34.32 540 99.20% – Ishak et al. (2020)
Ponceau
6R Dye
Methyl GrewiaVenusta Peel 2 0.5 – 150 – 85.00% 188.68 Ishak et al. (2020)
orange
Dye
Indigo Moringa Oleifera Seeds 5 0.5 – 150 – – 31.25 Ishak et al. (2020)
carmine
Dye
Methylene Carbonized watermelon 5.6 0.8 30 ◦ C 100 – 99% 200 Jawad et al.
Blue Dye (Citrullus lanatus) rind (2019)
Methyl Aspergillus iizukae 605EAN – – – 400 4320 84.90% – Noman et al.
orange (3days) (2020a)
Dye
Methyl red Aspergillus iizukae 605EAN – – – 400 4320 47.65% – Noman et al.
Dye (3days) (2020a)
Remazol Aspergillus iizukae 605EAN – – – 100 12,960 94.78% – Noman et al.
brilliant (9 days) (2020a)
blue R
Dye
Cr (III) Honeydew peel activated carbon 4.5 1.0 – 1000 40 83.49% 834.94 Yunus et al.
with H2SO4 (HDP-ACS) (2020)
Cr (III) Honeydew peel activated carbon 4.5 1.0 – 1000 40 88.8% 888.85 Yunus et al.
with H3PO4 (HDP-ACP) (2020)
Zn (II) Honeydew peel activated carbon 5.5 1.0 – 400 40 81.55% 326.19 Yunus et al.
with H2SO4 (HDP-ACS) (2020)
Zn (II) Honeydew peel activated carbon 5.5 1.0 – 400 40 84.13% 336.51 Yunus et al.
with H2SO4 (HDP-ACP) (2020)
Cd (II) Watermelon Rind 9.12 1.0 20 ◦ C 500 – 80% 40.16 Husein et al.
(2017)
Cu (II) Activated watermelon based 5 1.0 40 C◦
10 – 88% 31.25 Gupta and Gogate
biosorbent (2016)
Cu (II) Chitin 7 2.0 – 100 360 – 20.50 Sofiane and Sofia
(2015)
Cd (II) Chitin 7 2.0 – 100 360 – 13.27 Sofiane and Sofia
(2015)
Zn (II) Chitin 7 2.0 – 100 360 – 5.35 Sofiane and Sofia
(2015)

functional groups on the created biosorbent surfaces. There are several be undertaken for future applications.
mechanisms of biosorption for the removal of both inorganic and
organic compounds which are mentioned the most: electrostatic inter­ Declaration of competing interest
action, ion exchange, and complexation. Despite the impressive growth
in the development of different biosorbents, there are still many The authors declare that they have no known competing financial
remaining challenges associated with these materials, such as stability interests or personal relationships that could have appeared to influence
towards different pH, sorption capacity, and durability, which need to the work reported in this paper.

11
A.M. Elgarahy et al.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.clet.2021.100209.
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