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A Review of Fish Scales as a Source of Biosorbent for the Removal of Pollutants

from Industrial Effluents

Technical Report · January 2019

DOI: 10.13140/RG.2.2.20511.61604

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Eletta USEP: Journal of Research Information in Civil Engineering, Vol.16, No.1, 2019
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A Review of Fish Scales as a Source of Biosorbent

for the Removal of Pollutants from Industrial
Effluents
Omodele A. A. Eletta*1 and Joshua O. Ighalo2
1,2
Department of Chemical Engineering, Faculty of Engineering and
Technology, University of Ilorin, Ilorin, Nigeria,
1
modeletta@unilorin.edu.ng; modeletta@hotmail.com
2
oshea.ighalo@yahoo.com
*corresponding author

Abstract

Biosorbents prepared from fish scales has been used to treat wastewaters
containing heavy metals, dyes and pharmaceuticals. These pollutants have
been reported in effluents from pharmaceutical, textile, automotive battery
and tannery industries amongst others. Biosorption is a cheaper and more
environmentally friendly alternative to other treatment technologies including
the use very popular activated carbon adsorption. The aim of this review is to
catalogue the progress made over the past 15 years in the utilisation of fish
scales as biosorbents for the treatment of industrial effluents. Key domains
are in source fish species, biosorbent preparation technique, target impurities,
optimal levels of biosorption factors, equilibrium and kinetic best-fits and
thermodynamic findings. The biosorbents are generally prepared by a two-
stage chemical pre-treatment process. It is then dried, pulverised and sieved
and in some cases calcined. Fish scale biosorbents have been found to have
very good adsorption capacity for heavy metals, dyes and pharmaceutical
compounds and with excellent removal efficiencies (50-100% for heavy
metals and 78-90% for dyes). Optimal biosorption parameters vary
significantly for the different target impurities and is only consistent for pH
(acidic) and temperature (30-500C). Fish scale biosorption equilibrium is
always best fit to Langmuir or Freundlich isotherms with newer models
having poorer coefficients of determination. Fish scale biosorption kinetics is
best fit to the pseudo-second order model. The review also revealed that fish
scale biosorption is generally spontaneous and endothermic (for heavy metals
alone).

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Keywords
Waste management, Biosorption, Fish scale, Heavy metals, Dyes,
Pharmaceuticals

1. Introduction

Fish is a source of protein that is consumed in extremely large quantities not

only because it is cheaper than many other animal sources of protein, but
because nutritionists have classified it as a very safe source of animal protein
(white meat) also. Some are scally while others are without scales. So much
scale is produced from the sales of scaly fishes and, many studies have been
carried out on the use of these scales to add value to life while reducing the
ability to constitute nuisance when it is just discarded to the environment.

One of the recent trends in wastewater treatment by the adsorption is the

utilization of living and non-living biomass; this is known as biosorption
(Demirbas, 2008). Biosorption can be defined as the removal of substances
from solution by biological material (Goeffrey, 2008). Techniques and
mechanisms involved in the process have been examined (Amirnia, 2015;
Bailey et al., 1999; Ramachandra et al., 2006). Biosorption is different from
bioaccumulation (Zabochnicka-Świątek & Krzywonos, 2014). The former
describes the removal of heavy metals by the passive binding to non-living
biomass from an aqueous solution and the mechanism is not metabolically
controlled. In contrast, bioaccumulation describes an active process whereby
removal of metals requires the metabolic activity of a living organism (Abdi
& Kazemi, 2015).

Biosorption can be defined as the uptake of chemical species from aqueous

solutions onto biological materials via any of, biological, physical and
chemical mechanisms. An example is the ability of biological materials to
accumulate heavy metals from wastewater through metabolically mediated or
physico-chemical pathways of uptake (Abbas et al., 2014). It could also be
the passive binding of heavy metals to non-living cells (Abdi & Kazemi,
2015). The biosorption process can been used to remove heavy metals, dyes,
phenolics, and pesticides (Carson et al., 2009) from aqueous solutions.

A plethora of organic materials have been used for biosorption studies and
this includes; agricultural wastes (Sud et al., 2008), cherry leaves (Aathithya

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et al., 2014), crab shells (An et al., 2001), chitin (Anastopoulos et al., 2017),
egg shells (Bamukyaye & Wanasolo, 2017; Mutavdžić Pavlović et al., 2017),
some fruit shells (Hevira et al., 2015) and a host of others (Al-Othman et al.,
2012; A. Okoronkwo & Olasehinde, 2007; A. E. Okoronkwo et al., 2009;
Sekar et al., 2004). The use of fish scale in the preparation of biosorbents is
also very popular and a number of these have been used for different studies.
The scales of several fishes investigated by researchers for the preparation of
biosorbent includes Gadus morhua (Basu et al., 2006; Basu et al., 2007;
Rahaman et al., 2015), Tilapia nilotica (Huang, 2007; Zhe et al., 2014; Zhu et
al., 2013), Oreochromis niloticus (Neves et al., 2017; Ribeiro, Scheufele,
Alves, et al., 2018; Ribeiro et al., 2015; Ribeiro, Scheufele, Espinoza-
Quiñones, et al., 2018), Labeo rohita (Chakraborty et al., 2012; Iqbal et al.,
2011; Kondapalli & Mohanty, 2011; Mandal et al., 2015; Marrakchi et al.,
2016; Marrakchi et al., 2017; Nadeem et al., 2008), Catla catla (Das et al.,
2016; Kondapalli & Mohanty, 2011; Prabu et al., 2012; Srividya & Mohanty,
2009) among others. In some cases, the researchers were not specific on the
species of fish from which the scales were sourced (Bamukyaye & Wanasolo,
2017; Nielsen & Bandosz, 2016; Ooi et al., 2017; Stevens & Batlokwa,
2017). The study is an extensive review of the use of fish scale derived
biosorbents in removing pollutants such as heavy metals and dyes from
industrial effluents.

2. Source and Preparation Techniques of Biosorbent

Biosorbent from fish scales are usually easy to source and prepare. The major
source as reported by researchers is the market, fish industries and large
culinary establishments. Some of the scales are prepared and used directly,
others are impregnated with additives, calcined or used as source for deriving
hydroxyapatite. Table 1 presents a list of scally fish species that serve as
sources of scales for biosorbent preparation.

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Table 1 Source fish species for biosorbent preparation

Reference
Basu et al. (2006)
Basu et al. (2007)
Huang (2007)
Nadeem et al. (2008)
Amjad and Jamal (2008)
Srividya and Mohanty (2009)
Iqbal et al. (2011)
Kondapalli and Mohanty
(2011)
Chakraborty et al. (2012)
Liu et al. (2012)
Prabu et al. (2012)
Vieira et al. (2012)
Mota et al. (2012)
Kongsri et al. (2013)
Bajić et al. (2013)
Zhu et al. (2013)
Zhe et al. (2014)
Mandal et al. (2015)
Rahaman et al. (2015)
Ribeiro et al. (2015)
Uzunoğlu and Özer (2016)
Nielsen and Bandosz (2016)
Marrakchi et al. (2016)
Othman et al. (2016)
Das et al. (2016)
Marrakchi et al. (2017)
Neves et al. (2017)
Fish species
Gadus morhua (Atlantic cod) and
Lethrinus nebulosus (spangled emperor)
fish scales
Gadus morhua (Atlantic cod) fish scale
Tilapia nilotica fish scale
Labeo rohita fish scale
Lethrinus nebulosus fish scale
Catla catla fish scales
Exoskeleton of prawn (Nephrops
norvegicus) and Labeo rohita fish scales
Catla catla and Labeo rohita fish scales
Labeo rohita Fish scales
Ctenopharyngodon idella (grass carp) fish
scales
Catla catla fish scale
Leporinus elongates fish scale
Micropogonias furnieri (Corvina) fish
scale
Nano-crystalline hydroxyapatite from
Tilapia nilotica fish scale
Cyprinus carpio (carp) scales
Tilapia nilotica fish scale
Tilapia nilotica fish scale-based porous
carbon
Labeo rohita Fish scale derived
hydroxyapatite
Gadus morhua (atlantic cod) fish scale
Oreochromis niloticus fish scales
Dicentrarchus labrax fish scales
fish waste derived adsorbent
carbonized Labeo rohita fish scale
Mozambique tilapia fish scale
Catla catla fish scales
carbonized Labeo rohita fish scales
Orechromis niloticus fish scale

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Ooi et al. (2017) Mixed fish scale

Bamukyaye and Wanasolo
(2017)
Stevens and Batlokwa (2017)
Wen-Kuang et al. (2017)
Oreochromis mossambicus (Tilapia) fish
Ahmadifar and Koohi (2018)
Ribeiro, Scheufele, Alves, et
al. (2018)
Ribeiro, Scheufele, Espinoza-
Quiñones, et al. (2018)
fish scales
fish scale waste
hydroxyapatite scaffolds from
scale
Impregnated nano-magnetic Fe3O4 on
Rutilus kutum fish scale.
Orechromis niloticus (Nile tilapia) fish
scales
Orechromis niloticus (Nile tilapia) fish
scales

The fish scales are first washed with either tap (Bamukyaye & Wanasolo,
2017; Ooi et al., 2017; Rahaman et al., 2015), distilled (Chakraborty et al.,
2012; Kondapalli & Mohanty, 2011; Neves et al., 2017; Uzunoğlu & Özer,
2016) or de-ionised water (Basu et al., 2007; Das et al., 2016; Huang, 2007;
Stevens & Batlokwa, 2017) to remove dusts, dirt and other unwanted
particles. Washing with synthetic detergents (Amjad & Jamal, 2008).
Chemical treatment using an acid (Nadeem et al., 2008; Ribeiro et al., 2015),
base (Iqbal et al., 2011; Nadeem et al., 2008; Othman et al., 2016; Vieira et
al., 2012; Zhu et al., 2013), peroxide (Bajić et al., 2013) or a hypochlorite
(Iqbal et al., 2011; Ribeiro et al., 2015). Sometimes physical treatment by
applying heating alongside the chemical treatment is also employed (Das et
al., 2016; Nadeem et al., 2008; Ribeiro et al., 2015). In cases where chemical
treatment is employed, rinsing is also undertaken with the use of distilled
water. Sun drying (Kondapalli & Mohanty, 2011; Nadeem et al., 2008; Prabu
et al., 2012; Srividya & Mohanty, 2009), air drying (Huang, 2007; Rahaman
et al., 2015; Uzunoğlu & Özer, 2016) and oven drying (Bamukyaye &
Wanasolo, 2017; Neves et al., 2017; Ooi et al., 2017) has been reported.
Where no specific time was stated, scientific methodology is to terminate
drying when no further weight loss is noticeable. Some researchers did not
employ the use of any size reduction technique (Neves et al., 2017; Uzunoğlu
& Özer, 2016). Others utilised mortars (Nadeem et al., 2008; Othman et al.,
2016), mills (Liu et al., 2012; Ooi et al., 2017; Ribeiro et al., 2015), grinders
(Bajić et al., 2013; Prabu et al., 2012; Zhu et al., 2013) and pulverisers
(Amjad & Jamal, 2008; Iqbal et al., 2011; Stevens & Batlokwa, 2017).

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Sieving was done by a plethora of mesh sizes to obtain different particle size.
Several researchers undertook post-sieving or post-grinding chemical
treatment (Das et al., 2016; Stevens & Batlokwa, 2017). Passing the fish
scales through furnace to induce a compositional transformation/modification
of the fish scales has also been reported (Mandal et al., 2015; Marrakchi et
al., 2016; Marrakchi et al., 2017; Nielsen & Bandosz, 2016; Zhe et al., 2014).
This is a process called calcination (as opposed to carbonization for organic
materials). Fish scale is a calcium-rich compound and passing it through high
temperatures only serve to drive out the oxygen from the compound leaving
behind a deoxygenated compound of calcium.
Table 2. Summary of preparation techniques for biosorbent
Refere Washing and Pre-Treatment Preparation Technique
nce 1st stage 2nd stage Drying Grin Sieving
Proce Chemi Proc Chemi ding
ss cals ess cals
Basu Rinsi Deioni - - Oven - 35-40 µm
et al. ng sed drying
(2007) water at
650C
Huang Soaki Deioni - - Air - -
(2007) ng, sed drying
24hr, water for 2
rinsin days
g
Nadee Soaki 0.1M Was Deioni Sun Mec 150µm
m et ng HCl, hing sed drying hani particle
al. 2hr, H2SO4, water for 2 cal size
(2008) 300C, H3PO4, days, grin
100rp NaOH, Oven der
m Ca(OH drying befo
)2 , at re
Al(OH 700C pre-
)3 treat
ment
,
mort
ar

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after
pre-
treat
ment
Amjad Wash Synthe Post Post Vacuu Pulv 100 mesh,
and ing tic Pulv Pulveri m erise 150µm
Jamal for liquid erisa sation oven d by particle
(2008) 1hr deterge tion treatm drying hous size
(then nt, treat ent at ehol
Rinsi ment (0.05 300C d
ng (300 M elect
with C EDTA rical
distill for ) grin
ed 4hrs) der
water
)
Srividy Wash Water - - Sun Grin 100, 120,
a and ing drying ded 150, 200
Mohan for 2 (Baj and 240 µm
ty days, aj mesh
(2009) post- mod
pulveri el
sation GX7
oven )
drying
at
700C
for
2hrs
Iqbal Soaki 1mol/L De- De- Oven Pulv
et al. ng for NaOH mine minera drying erise
(2011) 24hrs ralis lisation at d
and ation with 800C
250C at 2mol/L for
(first 250C HCL, 8hrs
pre- , De- De-
washe pigm pigme
d entat ntation
with ion with

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distill at NaClO
ed 250C (1%,
water and w/v)
) 15mi
ns
(first
pre-
wash
ed
with
distil
led
wate
r in
both
case
s)
Konda Wash Distille - - Sun Grin 100, 120,
palli ing d drying ded 150, 200
and water for 2 (Baj and 240 µm
Mohan days, aj mesh
ty post- mod
(2011) grindi el
ng GX7
oven )
drying
at
700C
Chakra Wash Distille - - Sun Grin 100 -
borty ing d drying ded 125µm
et al. water for 2 particle
(2012) days, size
oven
drying
at
700C
Liu et Wash Water Was Distille Dried Crus 100 mesh
al. ing hed d hing
(2012) by thric water mill

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stirrin e
g for
5hrs
Prabu Wash Water - - Sun By 100-150
et al. ing drying mec mesh
(2012) repeat for 2 hani
edly days, cal
oven grin
drying der
at
700C
Vieira Imme NaOH 60mi Distille oven Mixi 100µm
et al. rsed sol ns d drying ng mesh
(2012) for (pH unde water, at with
4hrs 9.0) r ultraso 600C wate
at ultra und for r at
ambie soun 6hrs. 4000
nt d, post- rpm
condit 10mi grindi for
ions ns ng 6s
with oven
doub drying
le- at
distil 600C
led for
wate 24hrs
r
Mota Wash water - - Drying - -
et al. ing at
(2012) 350C
for
12hrs
Bajić Sonic 5% Tripl De- Dried Grin Sieved to
et al. ation H2O2 e ionised ded 100 ±50µm
(2013) rinsi water grains
ng
Zhu et Heate NaOH Rins Water Drying Grin Sieved
al. d in solutio ing at ded through
(2013) an oil n 500C 160 mesh

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bath
Raham Wash Tap Rins Distille Air - -
an et ing water ing d drying
al. Water at
(2015) 250C
for
24hrs
Ribeir Wash NaClO Was Distille Oven Tritu Tyler
o et al. ing (1%, hing d drying rated sieves 6,
(2015) w/v), Water at usin 12, 16, 32,
600C ga 100, 150
knife and 325
mill mesh
Ribeir 100rp 0.1M Was Distille Oven Tritu Tyler
o et al. m for HCl hing d drying rated sieves 6,
(2015) 24hrs Water at usin 12, 16, 32,
at 600C ga 100, 150
300C knife and 325
mill mesh
Uzuno Wash Distille - - Air Not Not sieved
ğlu ing d drying grin
and water for ded
Özer 48hrs
(2016) and
oven
drying
at
1100C
Marrak Wash Distille - - Oven - -
chi et ing d drying
al. water at
(2016) 600C
for
24hrs
Othma Left 15% Left Distille Oven Mort 100 mesh,
n et al. to NaOH to d drying ar 150µm
(2016) stand sol stan water at grin particle
for d for 600C der size
24hrs 24hr

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s
Das et Rinsi De- Post- water Post- Cutti -
al. ng ionised cutti cutting ng
(2016) water ng oven into
ther drying 0.5c
mal at m×
treat 500C 0.5c
ment over m
600C night piec
for es
10mi
ns
Neves Wash Distille - - Oven Not Not sieved
et al. ing d drying grin
(2017) water at ded
600C
Ooi et Wash Tap Rins De- oven Ultra 0.2mm ring
al. ing water, ing ionised drying - sieve, then
(2017) then water at centr vibratory
hot 500C ifuga laboratory
water for l shaker, size
48hrs mill range of 63
- 100µm
Bamuk Wash Tap Rins De- oven Mec 300 -
yaye ing water ing ionised drying hani 600µm
and water at cal mesh
Wanas 400C grin
olo der
(2017)
Steven Wash De- Post- De- Sun Pulv 63 - 200µm
s and ing ionised sievi ionised drying erise mesh
Batlok water ng water for d at
wa wash 48hrs. 400r
(2017) ing, post- pm
post- sievin for
sievi g oven 90mi
ng drying ns
treat at
ment 65±50

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with C for
vine 6hrs
gar
Ribeir Wash Distille - - oven - -
o, ing d drying
Scheuf water at
ele, 600C
Alves,
et al.
(2018)

3. Target Impurities

Biosorbents prepared from fish scales has been used to treat polluted
wastewaters containing heavy metals, dyes and pharmaceuticals.
These pollutants have been reported in effluents from pharmaceutical
(Chandrakanth et al., 2014; Deschamps et al., 2012; Gadipelly et al., 2014;
Pillai, 2016), textile (Chakraborty et al., 2012), automotive battery (Ribeiro,
Scheufele, Alves, et al., 2018; Ribeiro, Scheufele, Espinoza-Quiñones, et al.,
2018) and tannery (Bamukyaye & Wanasolo, 2017) industries. Heavy metals
examined in biosorption studies include lead, Cobalt, Copper, Cadmium,
Manganese, Zinc, Nickel, Chromium, Iron, Selenium and Arsenic. As
revealed by table 3, fish scale derived biosorbents perform excellently well in
removing heavy metals from aqueous solutions with most of the reported
removal efficiencies lying above 50%.

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Table 3. Heavy metals in biosorption studies

Reference Metal Optimum Method of Optimum
Adsorption Determining Removal
Capacity Adsorption Efficiency
(mg/g) Capacity (%)
Basu et al. Pb, - - 95
(2006)
Co - - 70

Basu et al. Pb - - 100

(2007)
Huang (2007) Cu - - 97.2
Nadeem et al. Pb 472 Experiments -
(2008)
Amjad and Pb - - 97
Jamal (2008) Cd - - 93
Cu - - 78
Mn - - 50
Zn - - 57
Ni - - 25
Cr - - 63

Srividya and Cr 27.1 Experiments 61

Mohanty
(2009)
Kondapalli Cr - - -
and Mohanty
(2011)
Liu et al. Ni 120.9 Experiments -
(2012)
Prabu et al. Cr, Fe, - - -
(2012) Co, Pb,
Zn, Cd,
Mn, Ni
Kongsri et al. Se - - -
(2013)

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Bajić et al. Pb 62.5 Langmuir 94

(2013) Isotherm
Cd 69.0 Langmuir 98
Isotherm
As 32.1 Langmuir 71
Isotherm
Mandal et al. Cu 209.732 Langmuir 91.77
(2015) Isotherm
Rahaman et As - - -
al. (2015)
Uzunoğlu and Cu 127.16 Langmuir -
Özer (2016) Isotherm
Othman et al. Zn - - 85
(2016) Fe - - 59
Das et al. Cu 79.35 Langmuir -
(2016) Isotherm
Bamukyaye Cr 27.27 Langmuir 50
and Wanasolo Isotherm
(2017)
Stevens and Pb - - 81.97
Batlokwa Zn - - 80.37
(2017)
Wen-Kuang Pb 344.8 Langmuir 99.9
et al. (2017) Isotherm
Ahmadifar Cu 61.73 Langmuir 76.5
and Koohi Isotherm
(2018)
Ribeiro, Zn 15.38 Langmuir- -
Scheufele, Freundlich
Alves, et al. Isotherm
(2018)
Ribeiro, Fe, Zn, - - -
Scheufele, Pb
Espinoza-
Quiñones, et
al. (2018)

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A number of pharmaceutical compounds and dyes have been studied using

fish scale derived biosorbent. The pharmaceutical compounds include Di-
chlorophenol (Mota et al., 2012), Sulfa-methoxazole and trimethoprim
(Nielsen & Bandosz, 2016). Dyes include methylene blue (Chakraborty et al.,
2012; Marrakchi et al., 2017; Zhe et al., 2014), acid yellow dye, remazol
yellow red and blue (Vieira et al., 2012) and a host of others. The adsorption
capacity for dyes and pharmaceuticals is higher than for heavy metals and
removal efficiencies range between 78-90% for dyes. Table 4 gives a
summary of the target impurities for fish scale biosorption studies for non-
metal pollutants.
Table 4 Other pollutants in biosorption studies
Reference Target Optimum Method of Removal
impurity Adsorption Determining Efficiency
Capacity Adsorption Capacity (%)
(mg/g)
Iqbal et al. Acid - - -
(2011) yellow
dye
Chakrabor Crystal 74.4 Langmuir Isotherm -
ty et al. violet
(2012) Methylen 58.7 Langmuir Isotherm -
e blue
Vieira et Remazol - - -
al. (2012) Yellow,
Remazol
Blue and
Remazol
Red
Mota et al. Di- - - -
(2012) chloro-
phenol
Zhu et al. Ponceau 134.4 Pseudo-second order 78
(2013) 4R kinetics
Zhe et al. Methylen 1050.72 Langmuir Isotherm -
(2014) e blue
Ribeiro et Reactive 241.20 Langmuir Isotherm -

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al. (2015) blue 5G

dye
Nielsen Sulfa- - - -
and methoxa
Bandosz zole,
(2016) trimetho
prim
Marrakchi Reactive 114.2 Langmuir Isotherm 95
et al. orange
(2016) 16 dye
Marrakchi Methylen 184.4 Langmuir Isotherm -
et al. e blue
(2017)
Neves et Reactive 272.39 Langmuir Isotherm -
al. (2017) blue 5G
dye
Ooi et al. AB113 157.3 Langmuir Isotherm 90
(2017) dye

4. Factor Optimisation

Biosorption is similar to adsorption hence the factors affecting the process is

the same as those for conventional sorption onto adsorbents. Some of these
factors are temperature, pH, biosorbent dosage, initial pollutant
concentration, agitation time, agitation speed, biosorbent particle size and
surface area amongst others. The nature and inherent characteristics of the
fish scales to be used for the biosorption has an effect on the process. Pre-
treatment processes are often developed to alter/affect some of these inherent
properties of the materials to favour the adsorption process. These includes
pulverizing, grinding, boiling, autoclaving, acid and alkali treatment among
others. Biomass can be considered as natural ion-exchange materials which
mainly contain weakly acidic and basic groups. Therefore, pH of solution
influences the nature of fish scale binding sites and metal solubility; it affects
the solution chemistry of the metals, the activity of the functional groups in
the biomass and the competition of metallic ions.

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The concentration of biosorbent per batch adsorption process has a

significant effect on the amount of the chemical compound adsorbed. At
lower concentrations, percentage of metal uptake by adsorbent is higher than
at higher concentration (Abbas et al., 2014). This is could be because, higher
concentrations restrict the access of metal ions to the binding sites. The initial
concentration of the chemical species to be adsorbed is another significant
factor in the process. Metal uptake increases with increasing concentration
due to the presence of a greater mass transfer driving force. The equilibration
time of the process is another factor because mass transfer to the pores of the
biosorbent can be incomplete if equilibrium is not achieved between the
biosorbent and the aqueous medium. Also, the smaller the size of the
particles, the larger the total surface area of the biosorbent. A high surface
area indicates a higher adsorption capacity.
Table 5. Summary of optimum parameters for biosorption
Reference Pollut Time pH Agitation Biosorb Temperature
ant (Mins) Speed -ent (0C)
(RPM) Dosage
(g/L)
Nadeem et Pb - 3.5 50-400 - -
al. (2008)
Amjad and Pb 60 5.5 - - -
Jamal Cd 75 7 - - -
(2008) Cu 150 6 - - -
Ni 125 7.5 - - -
Zn 150 6 - - -
Fe 150 5 - - -
Cr 150 5 - - -
Mn 150 8.5 - - -
Srividya Cr 180 1.0 200 0.05
and
Mohanty
(2009)
Iqbal et al. Acid - 3 - - 30
(2011) yello
w dye
Kondapalli Cr 180 - - - -
and

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Mohanty
(2011)
Chakrabort Cryst - 9 - 1 40
y et al. al
(2012) Violet
Meth - 8 - 2 40
ylene
Blue
Liu et al. Ni 60 6.3 - - 30
(2012)
Prabu et al. Cr, 300 7 - 0.05 -
(2012) Fe,
Co,
Pb,
Zn,
Cd,
Mn,
Ni
Kongsri et Se - 5 - 0.15 -
al. (2013)
Bajić et al. Pb - 7 - - 30
(2013) Cd - 6 - - -
As - 4 - - -
Zhu et al. Ponce 25 7.5 - 0.24 -
(2013) au 4R
Zhe et al. Meth - 11 - - -
(2014) ylene
blue
Mandal et Cu 40 8 - - -
al. (2015)
Ribeiro et React - 2 - - -
al. (2015) ive
blue
5G
dye
Uzunoğlu Cu - 3 - 1 45
and Özer
(2016)
Marrakchi React - 9 - - 50

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et al. ive
(2016) orang
e 16
dye
Ooi et al. AB11 60 6 - 4 -
(2017) 3 dye
Bamukyay Cr -- 6.8 - 0.5 -
e and
Wanasolo
(2017)
Stevens Zn, 62.37 7.52 - 0.77 -
and Pb
Batlokwa
(2017)
Wen- Pb 20 - - - -
Kuang et
al. (2017)
Ahmadifar Cu 180 6 - - 45
and Koohi
(2018)

It can be observed that for heavy metal biosorption, acidic pH conditions are
optimum for metal uptake. Only Stevens and Batlokwa (2017), Mandal et al.
(2015) and Amjad and Jamal (2008) (for Mn) reported optimal basic pH
conditions for metal uptake. The non-metallic pollutants show a wider range
of optimum pH. Reported Optimum time varies greatly because equilibration
does not only depend on time but also on how the agitation speed. Hence a
study done at a higher rpm will invariably have a lower equilibration time
and vice versa.
Dosage cannot be generalised since it also depends on particle size such that,
the key variable is the number of active sites or functional complexes for
biosorption. Smaller particle sizes will require less dosage and larger
particles sizes will require more dosage to demonstrate an equal removal
efficiency. Optimum temperature for biosorption always lies somewhere
between 30 and 500C.

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5. Fish Scale Biosorption Equilibrium and Kinetics

As revealed in table 6, biosorption experiments most often correlates with
Langmuir and Freundlich equilibrium isotherms models. However, Ribeiro,
Scheufele, Alves, et al. (2018) reported Langmuir-Freundlich equilibrium
isotherms model as this best fit in their study. Biosorption kinetics is
according to pseudo-second order kinetics. However, Intra-particle diffusion
(Kongsri et al., 2013), generalised Elovich (Ribeiro, Scheufele, Alves, et al.,
2018) and pseudo-second first order (Kondapalli & Mohanty, 2011) has been
reported as best fit.

Table 6. Summary of Equilibrium and Kinetics for fish scale biosorption

Reference Target Best fit Equilibrium Best fit Kinetic
impurity Model and Parameters Model and
Parameters
Nadeem et Pb Freundlich Pseudo-second order
al. (2008) qmax= 181.81, KF= qe= 181.81mg/g, K2=
0.004384mg/g, R2= 0.004384g/mg min,
0.9447, 1/n= 0.5392 R2= 1.00
Amjad Cd Freundlich -
and Jamal KF= 0.00331µg/g, R2=
(2008) 0.9906, 1/n= 1.78
Pb Freundlich -
KF= 0.00457µg/g, R2=
0.9923, 1/n= 1.57
Srividya Cr Freundlich (400C) Pseudo-second order
and KF= 2.3147mg/g, R2= qe= 0.9939mg/g, K2=
Mohanty 0.9917, 1/n= 0.2403 0.0023g/mg min, R2=
(2009) 0.9939
Iqbal et al. Acid Langmuir -
(2011) yellow qmax= 0.0113mg/g, KL=
dye 1.1675L/mg, R2=
0.9132,
Kondapall Cr Freundlich (400C) Pseudo-first order
i and KF= 2.3147mg/g, R2= (400C)
Mohanty 0.9917, 1/n= 0.2403 qe= 3.6255mg/g, K1=
(2011) 0.0234min-1, R2=

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0.9708
Chakrabor Crystal Langmuir (400C) Pseudo-second order
ty et al. violet qmax= 74.5mg/g, KL= (400C)
(2012) 0.629L/g, R2= 0.998, qe= 72.04mg/g, K2 =
0.0079g/mg min, R2=
0.999
Methylene Langmuir (400C) Pseudo-second order
blue qmax= 58.68L/mg, KL= (400C)
0.67L/g, R2=0.999, qe= 57.46mg/g, K2 =
0.0962g/mg min, R2=
0.999
Liu et al. Ni Langmuir -
(2012) qmax= 120.9mg/g, R2=
0.9877,
Kongsri et Se Freundlich Intra-particle
al. (2013) KF= 2.12mg/g, R2= diffusion
0.9128, 1/n= 0.25 C= 0.048mg/g, Kdif=
0.021 mg/(gmin)1/2,
R2= 0.9627
Bajić et al. Pb Langmuir (200C) Pseudo-second order
(2013) qmax= 55.4mg/g, KL= qe= 34.05mg/g, K2=
1.15L/mg, R2= 0.995, 1.1050g/mg min, R2=
0.998
Cd Langmuir (200C) Pseudo-second order
qmax= 64.4mg/g, KL= qe= 43.76mg/g, K2=
1.81L/mg, R2= 0.996, 0.4152g/mg min, R2
= 0.998
As Langmuir (200C) Pseudo-second order
qmax= 28.8mg/g, KL= qe= 31.31mg/g, K2=
2.32L/mg, R2= 0.992, 0.2778g/mg min, R2=
0.997
Zhu et al. Ponceau Freundlich (300C) Pseudo-second order
(2013) 4R KF= 40.879mg/g, R2= (300C)
0.9938, 1/n= 0.4623 qe= 122.35mg/g, K2=
0.008g/mg min, R2=
0.9978
Zhe et al. Methylene Langmuir (500C, pH Pseudo-second order
(2014) blue 11) (500C, pH 11)
qmax= 1283.91mg/g, qe= mg/g, K2=

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KL= 0.3054L/mg, R2= 0.042g/mg hr, R2=

0.9994, 0.9999
Mandal et Cu Langmuir Pseudo-second order
al. (2015) qmax= 209.732mg/g, (at initial Cu conc of
KL= 0.1003L/mg, R2= 50mg/l)
0.9999, qe= 0.000024mg/g,
K2= 200g/mg min,
R2= 0.9999
Uzunoğlu Cu Langmuir Pseudo-second order
and Özer qmax= 127.16mg/g, KL= (at initial Cu conc of
(2016) 0.2466L/mg, R2= 29.17mg/l)
0.9932, K2= 0.0013g/mg min,
R2= 0.9997
Marrakchi Reactive Freundlich (300C) Pseudo-second order
et al. orange 16 KF= 36.52mg/g, R2= (300C)
(2016) dye 0.965, n= 4.69 qe= 24.76mg/g, K2=
0.000259g/mg min,
R2= 0.979
Othman et Zn Langmuir Pseudo-second order
al. (2016) qmax= 72.993µg/g, KL= qe= 49.26µg/g, K2=
2.015L/µg, R2= 0.997, 0.001min-1, R2=
0.999
Fe Langmuir Pseudo-second order
qmax= 55.249µg/g, KL= qe= 25.45µg/g, K2=
0.004L/µg, R2= 0.990, 0.003min-1, R2 =
0.998
Das et al. Cu Langmuir (400C, linear) -
(2016) qmax= 72.46mg/g, KL=
0.0234L/mg, R2=
0.999,
Marrakchi Methylene Langmuir (500C) Pseudo-second order
et al. blue qmax= 214.40mg/g, KL= (25mg/L MB conc)
(2017) 16.42L/mg, R2= 0.972, qe= 22.29mg/g, K2=
0.380g/mg min, R2=
0.999
Ooi et al. AB113 Langmuir (300C) Pseudo-second order
(2017) dye qmax= 151.0mg/g, KL= (300C)
0.012L/mg, R2= 0.997, qe= 10.68mg/g, K2=
0.3229g/mg min, R2=

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0.9492
Bamukyay Cr Langmuir
e and
Wanasolo
(2017)
Ahmadifar Cu Langmuir Pseudo-second order
and Koohi qmax= 55.2486mg/g, (at initial Cu conc of
(2018) KL= 0.0485L/mg, R2= 50mg/l)
0.9943, qe= 8.05mg/g, K2=
0.0061g/mg min, R2=
0.9962
Ribeiro, Zn Langmuir-Freundlich Generalised Elovich
Scheufele, qmax= 15.38mg/g, b= α= 109.93mg/g hr,
Alves, et 0.04mg1-(1/n)L1/ng-1, R2= α2= 2.71×10-12mg/g
al. (2018) 0.964, n=0.81 hr, β= 0.34g/mg, R2=
0.981

6. Thermodynamics of Fish Scale Biosorption

Thermodynamic study of biosorption process of pollutants on fish scale was

undertaken by researchers to estimate the feasibility of the adsorption
process. The Gibbs free energy change ( ) values is used to determine the
spontaneity or otherwise of a process as, a negative value of imply a
spontaneous process. Enthalpy change provides information about the
exothermic or endothermic nature of the process and differentiate between
physical and chemical adsorption processes while the entropy change
predicts the magnitude of changes in the process reversibility. Table 7 reveals
that metal biosorption by fish scale derived biosorbent is spontaneous and
endothermic. It is more varied for dyes and pharmaceuticals. Biosorption is
also generally a spontaneous process. However, non-spontaneous biosorption
has been reported (Iqbal et al., 2011).

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Table 7. Summary of thermodynamics of fish scale biosorption

Reference Target Thermodynamic parameters
impurity
Temp
(0C) (kJ/mol) (kJ/mol) (J/molK)
Iqbal et al. Acid 30 4.3 - -
(2011) yellow dye
Kondapalli and Cr 40 -15.9514 15.1048 98.5042
Mohanty (2011)
Chakraborty et Crystal 40 -20.74 47.23 180.41
al. (2012) violet
Methylene 40 -14.35 50.21 171.26
blue
Vieira et al. Remazol 25 -20.7 -199.68 -599.40
(2012) Yellow
Remazol 25 -17.2 -83.28 -219.22
Blue
Remazol 25 -22.48 -120.87 -330.00
Red
Mota et al. Di-chloro- 25 - -536.7 to -
(2012) phenol -50.9
Bajić et al. Pb 20 -45.6 27.3 249
(2013) Cd 20 -40.7 18.5 202
As 20 -40.3 17.6 197
Zhu et al. Ponceau 30 -7.17 -22.96 -0.05
(2013) 4R
Zhe et al. Methylene 30 -13.87 8.97 75.41
(2014) blue
Marrakchi et al. Reactive 30 -0.76 18.51 63.16
(2016) orange 16
dye
Ooi et al. (2017) AB113 dye 30 -20.59 -33.21 -0.0417
Ahmadifar and Cu 35 -3.083 5.5024 27.8811
Koohi (2018)

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7. Conclusion

Biosorption is an effective and cheap treatment technology for effluent

treatment which does not require carbonisation hence the mass reduction in
the process is negligible. Researchers have extensively studied the
optimisation, equilibrium, kinetics and thermodynamics of the process. Some
key generalisations can be deduced from the review. Fish scale derived
biosorbents have been proved to be adequate in treating wastewaters polluted
with heavy metals, dyes and pharmaceuticals. The biosorbents have good
biosorption capacities for these pollutants and give excellent removal
efficiencies when used. Though optimal biosorption parameters vary, it was
deduced that optimal conditions for metal sorption is acidic pH and
temperature range of 30-500C. Fish scale biosorption equilibrium is either
according to Langmuir or Freundlich isotherms and the biosorption kinetics
is according to the pseudo-second order model. Fish scale biosorption for
metals is generally a spontaneous process which is endothermic and varied
for dyes and pharmaceuticals. In conclusion, the recent trend in the research
on fish scales as biosorbent is the study of methods to improve the adsorption
capacity and removal efficiency of pollutants. This is being explored through
derivation of hydroxyapatite scaffolds from the scales and impregnation of
scales with dopants.

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