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Recent advances in the treatment of dye-containing wastewater from

textile industries: Overview and perspectives

Shakiba Samsami, Maryam Mohamadi, Mohammad-Hossein

Sarrafzadeh, Eldon R. Rene, Meysam Firoozbahr

PII: S0957-5820(20)30571-1
DOI: https://doi.org/10.1016/j.psep.2020.05.034
Reference: PSEP 2267

To appear in: Process Safety and Environmental Protection

Received Date: 2 March 2020

Revised Date: 15 May 2020
Accepted Date: 18 May 2020

Please cite this article as: Samsami S, Mohamadi M, Sarrafzadeh M-Hossein, Rene ER,
Firoozbahr M, Recent advances in the treatment of dye-containing wastewater from textile
industries: Overview and perspectives, Process Safety and Environmental Protection (2020),
doi: https://doi.org/10.1016/j.psep.2020.05.034

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© 2020 Published by Elsevier.

Recent advances in the treatment of dye-containing wastewater from textile

industries: Overview and perspectives

Shakiba Samsamia, Maryam Mohamadia, Mohammad-Hossein Sarrafzadeha,*, Eldon R.

Reneb, Meysam Firoozbahrc

a
UNESCO Chair on Water Reuse, Biotechnology Group, School of Chemical Engineering,

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College of Engineering, University of Tehran, Iran.
b
Department of Environmental Engineering and Water Technology, IHE Delft Institute for

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Water Education, Westvest 7, 2601DA Delft, The Netherlands.
c
Department of Polymer Engineering, School of Chemical Engineering, College of

Engineering, University of Tehran, Iran.

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*Corresponding author:

Prof. Mohammad-Hossein Sarrafzadeh,

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aUNESCO Chair on Water Reuse, Biotechnology Group,

School of Chemical Engineering, College of Engineering,

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University of Tehran, Iran.

Email address: sarrafzdh@ut.ac.ir

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Tel: +98 216111218

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Graphical abstract

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Abstract
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Dye-containing wastewater should be treated effectively in order to prevent adverse effects on
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the environment and water resources. This review summarizes the recent dye removal

technologies from wastewater, such as biological methods, advanced oxidation process (AOP),
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electrocoagulation, adsorption, and membrane technology and nano-technology. The

performances, operating conditions, important process parameters, and the advantages and

disadvantages of different treatment systems are reviewed. Besides, in order to achieve

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efficient color removal, a large number of researches have also focused on hybrid treatment
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technologies. Among the different hybrid treatments, the MBR (membrane bioreactor) and the

PMR (photocatalytic membrane reactor) technologies have been discussed in this paper as

promising methods for color removal from textile wastewater. Regarding effective factors in

the PMR systems performance, photocatalytic nanoparticles have been discussed as a

prominent factor. Since not many review papers focused on these methods, this paper has been

2
prepared in a way to cover this deficiency and address mentioned methods more

comprehensively.

Keywords: Dye removal, Textile wastewater, Hybrid treatments, Membrane bioreactor;

Photocatalytic membrane reactor.

1. Introduction

Water, a valuable and mandatory factor for life, is covering 71% of the earth's surface. This

amount consists of 97.5% salty water and only 2.5% freshwater, with only 0.007% available

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for drinking. [1]. Industrial wastewater from the textile industries contains different types of

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dyes and other organic and inorganic pollutants. The discharge of effluents from different

industries resulted from the growing pace of industrialization has caused serious problems.
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Recently, more than 10,000 types of dyes are being produced in the world based on the Color
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Index, which leads to 700,000 tonnes of dye production [2].

Aquatic life can be in a horrible danger because of the presence of these dyes in water bodies.
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Reducing the dissolved oxygen (DO) level in water caused by blocking sunlight from the water

system and resisting photochemical reactions is one of the side effects of this presence. Dyes
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even increase Chemical oxygen demand (COD) and biochemical oxygen demand (BOD) levels

of water sources. According to a study that focused on textile effluent characterization, COD
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and BOD in the last decade were in the range of (150-30,000) mg L-1 and (80-6000) mg L-1 on

average, respectively [3]. Harmful effects on the environment and human health are resulted
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by this increase [4].

Recent studies show that some known carcinogens must be removed before the dye wastewater

release into the environment. Several researches have reported the mutagenicity of azo dyes

and the potential of causing cancers. Myslak et al. have presented that German painters

3
developed bladder cancer after longtime being in contact with azo dyes [5]. De Lima et al.

examined the effluent of a textile processing plant to determine the mutagenic and carcinogenic

potential of that. This effluent contained some dyes such as the CI Orange 37, CI Disperse

Violet 93, CI Disperse Blue 373, and three unknown fluorescent compounds [6]. Besides the

dyes, Mazzo et al. found 47 g L-1 of benzidine in the same sample which was analyzed in their

research and the Department of Health and Human Services (DHHS) and the World Health

Organization (WHO) have presented that benzidine as a human carcinogen [7]. Moreover, dyes

that are made from benzidine, such as Direct Black 38, Direct Blue 6, and Direct Brown 95,

are a cancer factor in humans. The DHHS has reported that Direct Black 38 and Direct Blue 6

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cause cancer in animals and WHO mentioned that Direct Black 38, Direct Blue 6, and Direct

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Brown 95 cause cancer in animals [8].

The major industries that are causing the release of dyes in the environment are shown in
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Fig. 1. Textile industry (54%) forms half of the existing dye effluents seen in the world-wide
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environment followed by dyeing industry (21%), paper and pulp industry (10%), tannery and

paint industry (8%), and the dye manufacturing industry (7%) [9].
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Fig. 1. Major industries that are causing the release of dyes in the environment [9].

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On the other hand, in compliance with a detailed study of Market Research Future (MRFR),

the global textile dyes market annually increases at a CAGR of 8.13% over the forecast period

of 2016-2023 (which is shown in Fig. 2). That would cause serious problems for the

environment and humans. So, this issue should be addressed properly.

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Fig. 2. The global textile dyes market over the forecast period of 2016-2023 [10].
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Recently, countless research papers have scrutinized several dye removal methods. Being able

to eliminate amounts of dye from wastewaters in a brief period, without causing secondary
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contamination, is considered as an ideal dye removal technology. Existing methods can be

categorized into three major treatment categories called biological, chemical, and physical
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treatments [11]. Adsorption, advanced oxidation (AOP), biological treatment, electrochemical

treatment, and membrane filtration are some of the important methods commonly using for dye
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removal. It cannot be directly addressed that which one is the best method since each method

has its advantages and limits concerning cost, efficiency, feasibility, and environmental impact.
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Till now, no technique capable of satisfactory treatment exists since the nature of effluents

from industries contains complexity. A combination of several treatments known as hybrid

processes is often used practically to gain the most efficient quality as well as the most

economical way [12].

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 Till now, numerous review papers have been published that each of them has their own

approaches. Many of them focused on biological treatments, while some of them had attended

to chemical or physical treatments. Also, a few numbers of them had presented hybrid

processes for the removal of dyes from textile effluents. As a means to clarify the approach of

this paper, Table 1 has been prepared, which reports recently published review articles in this

field and demonstrates their chief aims. As it turns out from this table, a majority of the studies

are about biological treatments, while it seems hybrid techniques insufficiently addressed in

recent years. It has been tried to make up this scientific research lack partly in this paper.

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Table 1. Recently published review articles in the field of dye removal from wastewater.

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Source title Year Aim References

Textile wastewater dyes: Toxicity 8132 Presented various methods to treat the textile ]31[
profile and treatment approaches wastewater and introduced biological
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treatments as the best alternative that can be
appropriate for eco-friendly treatment methods.
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Efficiency of various recent 8132 Highlighted enzyme biodegradation and ]31[
wastewater dye removal methods: A adsorption dye removal as one of the most
review efficient dye removal technologies nowadays.
Also, suggested the utilization of a combined
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adsorbent in order to have higher efficiency and

ability to remove dyes at a faster rate.

8132 ]31[
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Wastewater treatment and dyes Reviewed the optimum efficiency of diverse

removal using electrocoagulation types of bio-sorbents and natural inorganic
aided by natural biosorbents – A adsorbents under optimum conditions to remove
review dyes from contaminated water.
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Bioremediation of textile effluent for 8132 Presented potential of microbial processes for ]31[
degradation and decolorization of the dyes' mineralization.
synthetic dyes: A review
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Recent advancements in 8132 Evaluating the performance of bioremediation ]31[

bioremediation of dye: Current status as a utilitarian option for the dyes' treatment.
and challenges

Recent advances in microbial 8132 Summarized the enzymes identified, bacterial ]32[
remediation of textile azo dyes strains isolated, mechanism of action and
methods involved in dye's degradation.

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Recent advances in anaerobic 8132 Reviewed recent advances on high-rate ]31[
biological processes for textile anaerobic methods. Also summarized current
printing and dyeing wastewater limitations of these techniques, and indicated
treatment: A mini-review future research directions.

The efficacy of bacterial species to 8132 Reviewed the efficiency of bacterial species ]81[
decolorize reactive azo, (individual and consortia) to remove azo,
anthroquinone and triphenylmethane anthroquinone and triphenylmethane dyes from
dyes from wastewater: A review wastewater.

A critical review on recent 8132 Critically reviewed the adsorbents investigated ]83[
advancements of the removal of in the last decade for the textile effluent
reactive dyes from dyehouse effluent treatment and compared their capacities for
by ion-exchange adsorbents removing dyes.

Study of environmental concerns of 8131 Defined different technologies for color ]88[
dyes and recent textile effluents removal from industrial effluents. Also,
treatment technology: A review discussed disadvantages and advantages of
those techniques.

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A critical review on recent 8131 A detailed survey on the dye removal ]81[
developments in the low-cost technologies with special attention to select
adsorption of dyes from wastewater the efficient low-cost adsorbents which are

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alternative to the existing AC (activated
carbon).

Potential of fungal laccase in 8131 Presented recent developments in the synthetic ]81[
decolorization of synthetic dyes

Reduction of color intensity from 8131

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dyes' treatment using fungal laccases.

Focused on dye removal efficiency and ]81[

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textile dye wastewater using mechanism of various organisms.
microorganisms: A review

Improved bacterial-fungal 8131 Mainly focused on important factors in order to ]81[

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consortium as an alternative approach achieve higher efficiency also, the effect of

for enhanced decolorization and various physico-chemical conditions in
degradation of azo dyes: A review decolorization and degradation of azo dyes.
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Biodegradation of synthetic dyes of 8131 Centered on the involvement of bacteria in ]81[

textile effluent by microorganisms: utilizing dye molecules as a source of nitrogen
an environmentally and economically or carbon or both. Also, discussed the factors
sustainable approach which influence the bacteria's performance.
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Recent advances in textile 8131 Focused on literature on the microbial consortia ]82[
wastewater treatment using microbial application in the treatment of textile
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consortia wastewater, the mechanisms involved in

biodegradation of dye and how they can
influence dye removal efficiencies.

Treatments for color removal from 8131 Presented an analysis of different mechanisms ]81[
wastewater: State of the art involved in the various dye removal processes
and reported approximately 180 experimental
tests in this area case by case.

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Degradation of anthraquinone dyes 8181 Discussed the presence and remediation of ]11[
from effluents: A Review focusing on anthraquinone dyes from dyehouse effluents,
enzymatic dye degradation with focused on enzymatic processes.
industrial potential

Impact of textile dyes on public 8181 Focused on the environmental impact of the ]13[
health and the environment dyeing industry. While highlighting the existing
technologies as well as promising new ones for
dye removal from textile wastewater.

Recent advances in the treatment of
dye containing wastewater from
textile industries: Overview and
perspectives
8181 Summarizes the recent dye removal This article
technologies from wastewater with focusing on
hybrid treatments in order to achieve efficient
color removal. Among the different hybrid
treatments, more attends the MBR (membrane
bioreactor) and the PMR (photocatalytic
membrane reactor) as promising methods
technologies for color removal from textile

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wastewater.

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The present paper discusses these current techniques for dye removal from wastewater. The
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focal purpose of this study is to provide a review including (i) textile industry as one of the
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most remarkable source of releasing dye wastewater, (ii) diverse dye removal technologies,

(iii) discussion on different mechanisms, and (iv) present literature on PMR and MBR as
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promising hybrid treatments.

2. Textile operations
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Textile manufacturing contains different processes which the most common one consists of

desizing, scouring, bleaching, and dyeing [32]. After preparing a specific mixture of chemicals,
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dyestuff, and water in these processes, the environment is the first destination of the leftover
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mixtures (dye effluent). Besides, 85% of dye contaminant is discharged from the dyeing stage

[14]. Dyeing is defined to be the process of adding color to fibers. A large volume of water is

used in not only dyebath but also during the rinsing step [33]. Fig. 3 demonstrates a list of water

pollutants that may be produced at different steps of wet processing.

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Fig. 3. Schematic of operations involved in textile industry and some of the pollutant generated at

each level [34],[35].

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3. Dyes
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Color exists everywhere, from the clothes we wear to all the objects around us, whether they

are human-made or natural. Until the nineteenth century, natural resources were the origin of
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these colors. Vegetables like plants, trees, and lichen formed the major group of these origins,
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followed by insects and molluscs. Thousands of years of dye utilization demonstrate that only

a dozen or so have been used practically, which reflects the instability of natural dyes.
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Nowadays, more than 7,000 colorants exist, and in 1974, the world sales of synthetic dyes

achieved a huge number of £ 1,500 million [36]. A market intelligence company issued a report
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in 2019, entitled ‘Synthetic Dyes and Pigments Market by Segments’ which presented that in

2018 the global market for synthetic dyes and pigments extended to a value of $52.0 billion,
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which have increased 1.4% in compound annual growth rate (CAGR) since 2014 and this rate

of growth will continue to 2022. Besides, reported that the largest market for synthetic dyes

and pigments companies is Asia-Pacific, that 41.9% of the global market belongs to it. It is

followed by North and South America, Western Europe, the Middle East, and then the other

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regions. Afterward, Asia-Pacific and Africa will have the fastest growth rate among all regions

in this market [37].

Production of synthetic dyes has happened recently, which is being furthered in large scales

because of the rise in dye demand. Recently, different industries like textiles, cosmetics,

plastics, and printing use dyes in a considerable amount as a crucial ingredient in their products

[4],[38]. W. H. Perkin and Hofmann discovered Mauveine in 1856, which was an instant

success for dying silk, thus ‘Dyestuff Revolution’ started. The importance of Mauveine

increased when it was used for dyeing wool using tannic acid as a discovery by Perkin and

others. His noteworthy achievement made him be called ‘Founder of dyestuffs industry.’

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Perkin’s success made his component chemists pay heed to this industry which made them

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announce more significant discoveries in the post-mauveine era [32].

Type of dyes -p
The chromophores and the auxochromes are two essential components of dye molecules. The
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first one is in charge of producing the color and the second one is able to supplement the

chromophore, rendering the molecule soluble in water, and provide enhanced affinity (to
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attach) toward the fibers [39]. Basically, dyes are organic compounds which can attach

themselves to surfaces of fabrics to convey a color [4]. Various types of synthetic dyes exist,
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which can be classified based on their molecular structure, colors, and applications. Table 2

depicts the common classification for dyes [40],[41].

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Table 2. Various types of dyes and their applications [34],[35].

Type Applications Example

Acid Cosmetics, food, leather,

nylon, paper printing ink, silk,
wool

C.I Acid Blue 45

Basic Inks, medicine, modified

nylon, paper polyester

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Basic Orange 5

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Direct Cotton, leather, nylon,
rayon, silk, paper
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Mordant Anodized aluminium,

natural fibres, leather, wool
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Mordant Black 11
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Reactive Cellulosic, cotton, nylon,

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silk, wool

C.I Reactive Blue 19

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 Azo Acetate, cellulose, cotton,
rayon, polyester

Methylen Blue

Disperse Acetate, acrylic fibres,

cellulose, nylon, polyamide,
polyester, cotton, plastic

Disperse Blue 5

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Sulphur Cotton, leather, paper,

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polyamide fibres, rayon, silk

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Solvent Fats, gasoline, inks,
lacquers, lubricants, oils,
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plastics, stains, waxes

Solvent Red 146

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Vat Cotton, cellulosic fibres,

polyester-cotton, rayon, wool
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Vat Orange 15
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In some cases, solubility is the factor which dyes can be classified based on it. As an example,

acid, basic, direct, mordant and reactive dyes are considered as soluble dyes. Whereas, azo,

disperse, sulphur, solvent and vat dyes are some of the examples of insoluble dyes, as depicted

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in Fig. 4 [42]. Normally, cationic (all basic dyes), anionic, and non-ionic dyes are used in the

textile industry depending on their particle charge dissolution aqueous solutions [43],[44].

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Fig. 4. Classification of dyes based on solubility.

Azo dyes form the highest percentage of produced dyes among all dye types (65-70%), and it
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is the most used dye around the world [45]. The majority of synthetic aromatic dyes are azo

dyes (monoazo, diazo, triazo, and polyazo), which consist of one, two, three or more (N = N)
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groups which are connected to benzene and naphthalene rings substituting with some

functional groups, like triazine amine, chloro, hydroxyl, methyl, and nitro as well as sulphonate

[46]. Chemical structures of some azo dyes are shown in Fig. 5. Pharmaceutical, textile dyeing,

food, cosmetics, and paper printing are some of the applications of azo dyes. Textile industry

forms the majority of this application (80%) because of its low cost, high stability, and color

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variety [47]. It was estimated that nearly 10-15% of dyes in effluents are released into receiving

water bodies because these dyes go unbound with the textile fibres [48]. As an example, the

amount of water and dyestuff needed for dyeing 1 kg of cotton is consecutively 30-60 g and

70-150 L, and it was reported that more than 50% of used dyes were discharged directly and

indirectly in water sources [49],[50].

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Fig. 5. Chemical structure of (a) diazo dye Acid Red 151, (b) monoazo dye Acid Orange 7, (c)

polyazo dye Sirius Red F3B, and (d) triazo dye Direct Blue 71 [51].
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4. Dye removal technologies

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Equalization and sedimentation were the preliminary water purification processes used as dye

removal methods in the late 1990’s since there was no dye effluent discharge limit [52].
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Improvements were made after acceptable establishment of effluent release standards, which

caused by presenting more efficient dye removal techniques [53]. It is noteworthy to state that

discoloration and degradation have a clear distinction. In fact, discoloration refers to a process

of color loss from wastewater, which is the analysis object. Whereas the water still may be rich

in organic substance [54]. In the case of having an impact of parameters, such as TOC (total

14
organic carbon) and COD, the used technology is more accurate to be referred to degradation.

In the dye degradation process, larger dye molecules are chemically broken down into smaller

ones. Carbon dioxide, water, and mineral byproducts are the outcomes of this process [55].

Minimizing adverse effects on the environment, protecting consumers and users, and co-

operating with government and public concerns over the harmful effect of their products were

established as aims by the ETAD (Ecological and Toxicological Association of the Dyestuffs

Manufacturing Industry) in 1974. SEPTA (Scottish Environment Protection Agency) and the

Environment Agency (EA) for England and Wales, regulated these matters in Great Britain.

Governments, especially in more developed countries, enforce increasingly strict legislation

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concerning dye removal from industrial wastewater. For example, the UK has enforced a law

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declaring that no synthetic chemicals should be discharged into the marine environment. It has

been legislated to ensure that dye-wastewater is controlled by textile industries. European

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Community (EC) regulations are stepping into enforcing stricter legislations [52].
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With respect to legislation, there is still no international consensus regarding the release of

textile effluent, including Azo dyes, and there is no official document that lists the different
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limit about effluent applied in different countries [56]. Many developed countries, such as

Canada, the nations of the EU, the United States of America, and Australia oblige
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environmental legislation that establishes limitation laws. Morocco and Turkey have copied

the EU model, while Thailand has copied the US system. In other regions, including Pakistan,
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India, and Malaysia, the effluent contamination limits are not mandatory, and they are just

recommended. In most cases, azo dye limitations are not specified as a separate group from
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that of groupings such as ‘total dissolved solids’ concentration [57].

In the following sections, common methods, that have been applied for removing dyes from

wastewater will be discussed.

4.1. Biological processes for dye removal from wastewater

15
Biological treatment is a low-cost and environmentally friendly process that produces less

sludge. Needing a lesser amount of reagents, having an energy-saving nature and being

economical are some of the features of this treatment, that can lead to complete mineralization

of dyes [55]. In this treatment, the main procedure is the conversion of biodegradable wastes

into simpler and harmless species in a biological process. This method has significant

advantages because of various microorganisms adaptability in degrading various compounds

[4],[58]. There are two ways of dye decolorization for this treatment: (1) adsorption on the

microbial biomass and (2) dye biodegradation by microbial cells [58].

These processes are divided into two categories called aerobic and anaerobic process which

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both can be used for wastewater treatment [59]. The products of aerobic and anaerobic

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treatments contain carbon dioxide and biomass; moreover, water is another product for the

aerobic treatment and methane for the anaerobic treatment. Dye solutions can be treated in an
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eco-friendly in this method without high investment and costs [4]. Textile wastewater consists
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of various microorganisms such as fungi, algae, and bacteria, with the ability to degrade present

diverse dyes [34]. Another biological treatment in an enzyme system, which has some benefits
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that are elaborated in the following paragraphs.

Bacteria, algae, fungi, and yeast are some of the microorganisms that have the potential of
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transforming dyes molecule into less harmful forms [60],[61]. Cell wall components (lipids

and heteropolysaccharides) as attribution to this property of microorganism are composed of

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various functional groups including hydroxyl, amino, phosphate, carboxyl, and other charged

groups which they can cause great, attractive forces between the cell wall and azo dye [62].
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4.1.1. Bacteria-assisted biodegradation

Bacteria were found to be generic and comparatively more effective in comparison with other

forms of microbes [63]. Many researches are proposing a wide range of bacterial strains for

textile dye decolorizing [64], [65], that their effectiveness depends on their adaptability and

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their activities under certain environmental conditions [66]. Many bacteria, such as

Pseudomonas, Aeromonas sp., Bacillus, Shigella, Klebsiella, and Rhodococcus are capable of

biodegrading azo dyes efficiently [67], [68], [69]. Being easy to culture and growing faster in

comparison with other microorganisms are the main advantages of working with bacteria

which are well-fitted material to be used for mineralizing azo dyes finely [70]. Different groups

of bacteria run the process of biodegradation of azo dyes under normal anaerobic, aerobic, or

facultative anaerobic conditions. The first stage of the mechanism of bacterial degradation is

reductive cleavage of azo bonds (-N=N-), which happens with the help of azoreductase

enzymes [71].

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Fig. 6. Proposed mechanism of azo dyes degradation by bacteria [72].

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4.1.2. Algae-assisted biodegradation

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Algale require no preservation since their growth only mainly depends on sunlight and carbon

dioxide, which does not generate secondary waste product and also helps to and can remove

the nutrients from wastewater [73]. Algae-based processes are often easy, operational method

and most cheaper and environment-friendly in comparison with method among other

conventional treatment methods [74], [75], [76]. Algal biomass has also been used vastly as a

17
bio-sorbent, and its characteristics like binding ability and high surface area have made it

possess an excellent adsorption potential and electric force to attract contaminants from

wastewater [77]. Based on some researches, various types of present contaminants in

wastewater such as -OH, RCOO− , -NH2 and PO3−

4 are metabolized and get absorbed on the

algae surface [78]. Color elimination by algae consists of three major steps. The first step is

algae utilization of chromophores to harvest the algal biomass, CO2, and H2O; then the non-

chromophore material are formed from chromophore material alteration in the second step; and

third, algal biomass absorbs the resulting chromophore [79]. Table 3 presents some recent

studies on biodegradation of dyes by algae.

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Table 3. Some recent studies on biodegradation of dyes by algae.

Algae Dye Dye removal Dye concentration References

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(mg L-1)
Monolithic algal green powder Crystal Violet 90.3% 5, 10, 15, 20 [80]
(MAGP), fabricated based on Methylene Blue 93.4% 5, 10, 15, 20
Enteromorpha flexuosa

Chlorella vulgaris Reactive Black 5

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>90% 100 [81]
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Reactive Black 5 >90%
Disperse Red 1 >90%

Spirulina platensis Indigo Blue >90% 25, 50, 75, 100 [82]
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4.1.3. Fungi-assisted biodegradation

A fungal culture can accelerate its metabolism to change the environmental conditions, and
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their existence lingers to this ability [83]. In this case, intra- and extracellular enzymes help in

metabolic activity. Enzymes like lignin peroxidase (LiP), manganese peroxidase (MnP) and
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laccase can make a suitable situation for dye degradation in textile wastewater [84].

Biodegradation of dyes through fungal strains results in the breakdown of the dye molecule

and consequently detoxification of harmful dyes [85]. Recently, several investigations on

fungal for color removing purposes have been furthered to be an alternative for present physical

and chemical techniques [86],[87],[88]. Industries containing Polycyclic aromatic hydrocarbon

18
(PAH) like textile, pulp, and paper industry can use Phanerochaete chrysosporium for effective

pollutants degradation [89]. Table 4 presents some recent studies on biodegradation of dyes by

fungi.

Table 4. Some recent studies on biodegradation of dyes by fungi.

Fungi Dye Dye removal References

Trametes versicolor Methyl Red 91% [83]

Reactive Blue 220 80%

Achaetomium strumarium Acid Red 88 99% [90]

Cylindrocephalum aurelium RY06 Mordant Orange-1 85% [91]

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4.1.4. Yeast-assisted biodegradation

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Some researches show the efficient performance of yeast species as dye adsorbents which are

capable of uptaking high dye concentration [92]. Although only a few studies have investigated
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the decolorization and degradation ability of yeasts, they can be used as a substitute for deleting

dyes in the textile industry because of its rapid growth like bacteria and its capacity to sustain
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in adverse environmental conditions even at low pH [72], [62]. Known yeast species with dye

removal abilities are mainly ascomycetous, including some belonging to Candida,

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Saccharomyces, Kluyveromyces, and Debaryomyces genera. Among basidiomycetous,

Trichosporon and Rhodotorula are the most promising genera [93]. Noticeable dye removal
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from diverse dyes caused by Pseudozyma rugulosa Y-48 and Candida krusei G-1 made these

two novel strains to be selected and identified among 44 yeast strains tested for permeability
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to destroy dyes. P. rugulosa Y-48 and C. krusei G-1 removed the Reactive Brilliant Red K-2BP

(200 mg L-1), with the efficiency up to 99% dye elimination after 24 h [94]. More studies show

that biodegradation proceeded primarily the decolorization of the dyes tested [46].

4.1.5. Enzyme-assisted biodegradation

19
Enzymes are not the first choice in wastewater treatment due to their cost in pure form.

However, industrial and not too purified enzymes, as reliable, low-priced, efficient, and

regenerable agents, also exist in a liquid form [95]. It is reported in a recent research that

enzymes have the highest efficiency in eliminating dyes [14]. Enzymes convert stubborn

pollutants into products or use precipitation process to remove them from wastewater [96].

Enzymes became reputable for their easy availability and green chemistry. They can be used

in numerous applications as an upcoming technology [97],[14]. Laccases and azoreductases

have shown their great potential for azo dyes degradation and enzymatic decolorization.

Laccases also have a great potential to decolorize a vast range of known industrial dyes

of
[98],[99].

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Fig. 7. Proposed mechanism for laccase degradation of Indigo dye [100].

21
4.2. Chemical processes for dye removal from wastewater

Regarding the theory of chemistry, dye removal is considered as chemical treatments. These

technologies are usually more expensive in comparison to biological and physical treatments

except for electrochemical degradation treatment. Some of the disadvantages of chemical dye

removal methods, which has made them unattractive for commercial use, are requiring proper

equipment, high electrical energy for reactors and also consuming a considerable amount of

chemicals as reagents [35],[101]. Toxic secondary pollution followed by chemical dye removal

process is another unwanted deficiency of this treatment which presents an additional disposal

problem [14].

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4.2.1. Advanced Oxidation Processes (AOPs)

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Glaze et al. scrutinized advanced oxidation processes (AOPs) and defined them as water
-p
treatment technology applicable under the specific condition of temperature and pressure [102].

This process is based on the in-situ generation of a strong oxidizing agent like hydroxyl radicals
re
(OH • ), which effectively decontaminate waters at a sufficient concentration. AOPs are being
lP

renowned increasingly based on their vast applications in research works [103],[104],[105].

Various process technologies such as ozonation, Fenton, photo-Fenton, photocatalysis,

electrochemical oxidation, ultrasound, plasma, and UV-based have been investigated for
na

utilizing this potent oxidizing agent. They could be applied either individually or coupled with

each other. These treatments, those including UV irradiation and ozonation, in particular, have
ur

already been used commonly for operation in treating drinking water and wastewater at full-
Jo

scale [106].

In the following reaction set, the formation of OH • radicals can be observed as a result of the

photolysis of ozone in water. Eq. (1) corresponds to the initiation step, Eqs. (2) and (3) to the

propagation steps and Eqs. (4) and (5) to the termination steps [107].

O3 + H2 O + hv → 2 OH • + O2 (1)

22
O3 + OH • → HO•2 + O2 (2)

O3 + HO•2 → OH • + 2 O2 (3)

OH • + HO•2 → H2 O + O2 (4)

2 OH • → H2 O2 (5)

Also, hydrogen peroxide can absorb UV irradiations at a specific wavelengths ranging. The

following chain mechanism shows how OH • radical forms in this situation [107]:

H2 O2 + hv → 2 OH • (1)

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OH • + H2 O2 → H2 O + HO•2 (2)

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HO•2 + H2 O2 → OH • + H2 O + O2 (3)

OH • + HO− •
2 → HO2 + OH
−
(4)

2 HO•2 → H2 O2 + O2
-p (5)
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OH • + HO•2 → H2 O + O2 (6)
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Fenton method as the most practical AOPs, is a mixture of a soluble iron (II) salt and H2 O2 ,

known as the Fenton’s reagent, is applied for degrading and destroying stubborn organic
na

pollutants [108],[109]. Recent studies have shown that the formation of hydroxyl radical is the

initial stage of Fenton process, regarding the reaction (1), and could be applied to the
ur

degradation of various organic pollutants like dye molecules [107].

Fe2+ + H2 O2 → Fe3+ + OH • + OH −
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(1)

In addition to the above reaction, in the photo-Fenton process, the hydroxyl radical formation

also occurs by the following reactions [110]:

H2 O2 + UV→ 2 OH • (2)

23
Fe3+ + H2 O + UV→ OH • + Fe2+ + H + (3)

The photocatalysis process has been presented by many researches for OH • production along

with textile-waste degradation, which is potent for a maximum of 90% dye removal with

modifications [111]. Semiconducting materials like TiO2 and ZnO can be used as photocatalyst

for generating holes and free radicals, which leads to dye degradation. Fig. 8 peresents the

mechanism of radical generation in a photocatalytic process. Holes, as the oxidizing agents,

form mineralization products and OH • by organic compounds' oxidation. Electrons, as the

reducing agent, form superoxide [112].

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Fig. 8. Schematic diagram of photocatalytic degradation of dye [113].

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Ultrasound is one of the advanced oxidation processes. The following chain of reactions shows

the sonication of pure water which leads to the formation of radicals [114]:

H2 O + ))) → OH • + H • (1)

OH • + H • → H2 O (2)

24
OH • + OH • → H2 O2 (3)

H • + H • → H2 (4)

Also, a new AOPs based on the electrochemical technology (EAOPs) have been developed in

recent years for wastewater treatment approaches. Using electron as a clean reagent, has made

an environmental-friendly technique. In the EAOPs, OH • radicals are produced at the surface

of anode through heterogeneous processes like photoelectrocatalysis and anodic oxidation

(AO), OH • radicals are generated in the bulk solution through homogeneous processes like

photoelectro-Fenton, sonoelectrolysis and electro-Fenton (EF) [115].

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Hydroxyl radical as a radical containing 2.8 V (at pH 0) to 1.95 V (at pH 14) range of oxidation

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potential, is the most reactive oxidizing agent vs. saturated calomel electrode (SCE) for

wastewater treatment [116]. Owing to the fact that HO• can react by hydrogen-atom abstraction

(which is less prevailing) while SO•−

-p
4 prefers the electron transfer reactions, the sulfate radicals
re
−
have a longer half-life. S2 O2−
8 and HSO5 which operate as oxidants can be activated by light,

heat, or by catalyst usage to produce SO•−

4 as shown in Eqs. (1)-(3). Moreover, to compare with
lP

classic AOP, these radicals include a more extensive pH range of productive usage [117].

−
S2 O2− •−
8 / HSO5 + hv → 2 SO4 (1)
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−
S2 O2− •−
8 / HSO5 + ∆ → 2 SO4 ; Ea = 33.5 kcal/mol (2)
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−
S2 O2− − •−
8 / HSO5 + 2 e → 2 SO4 (3)
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Eq. (4) and (5) show that how sulfate radicals can be decomposed to generate HO• when present

in aqueous medium or at basic pH [118]:

2 SO•− • −
4 + H2 O → HO + HSO4 (4)

SO•− − • 2−
4 + OH → HO + SO4 (5)

25
Extensive various activation techniques, as well as oxidant generation, can productively be

used for a number of different mechanisms for organic destruction as technologies for AOPs.

Fig. 9 demonstrates applied processes for utilizing radical in hydroxyl radical-based AOPs.

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Fig. 9. Hydroxyl radical-based AOPs.

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4.2.2. Coagulation-Flocculation

Coagulation and flocculation, as a vital process for the removal of coloring substances in
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wastewater, are furthering a process that destabilizes the solid particles which are dispersed in

water by reducing their surface charge, which results in being gathered to form larger particles.

Coagulation, flocculation, and sedimentation are the three steps of this procedure. Firstly,

coagulants are added in a violent mixing condition. Secondly, the charge of finely dispersed

particles is reduced, or they are neutralized because of the coagulants act. Then, flocculants are

26
mixing gently to gather fine particles together and form larger particles. Finally, large particles

are removed by sedimentation afterwards [119],[4]. Coagulants are materials such as metal

salts and polymers, and flocculants are polymers causing flocs aggregation enhancement to

create larger elements for easier separation [29],[4]. Some natural materials that have been

reported as highly efficient coagulants specifically in dye removal from effluents are:

Tamarindus Indica, Moringa oleifera, Musa genus, and Azadirachta indica [120]. Based on a

recent research, several chemical coagulants that used in the coagulation-flocculation process

are: aluminium sulphate solution (Al2 (SO4)3.18H2O), MO-KCl (the extract from the Moringa

oleifera Lam. seeds in potassium chloride), MO-NaCl (the extract of Moringa oleifera Lam.

of
seeds in sodium chloride) [121].

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4.2.3. Electrochemical treatments

4.2.3.1. Electrocoagulation (EC) -p

This method is used for removing organic contaminants from wastewater. Two metal
re
electrodes use this direct power source for being immersed in wastewater. The coagulant

particles are formed in situ. Aluminum or iron, as metal anodes act as catalyst and coagulant
lP

agent and hydrogen gas is evolved at cathode [122]. The flocculated species are floated by the

assistance of the hydrogen gas. Electrolytic oxidation and reduction occurring at the suitable
na

electrode in an electrochemical reactor generate the coagulant. Colorless, clear, and odorless

water is generated as a result of this process. Besides, operable in ambient condition,

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effortlessness, able to handle the considerable volume, no need of chemical materials using,
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generating lower sludge, high reaction rate, cost-effective, and environment-friendly are certain

features displayed by wastewater [123],[124]. Fig. 10 schematically presented the mechanism

of this treatment.

27
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Fig. 10. Electrocoagulation mechanism [125].

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4.2.3.2. Electro-Fenton (EF)

-p
Organic substances are removed in two stages called oxidation and coagulation, which is

known as electro-Fenton, a development in the hybridization of electrolysis and Fenton’s

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degradation reaction. It can be considered as one of the most reputable electrochemical AOPs
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[126]. Better control of the process, lack of secondary pollutants, no necessity to the use of

harmful reagents are some of the advantages of using electro-Fenton process, which results in

its consideration as an environmentally friendly wastewater treatment method [127].

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4.2.3.3. Anodic oxidation (AO)

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Anodic oxidation destroys pollutants in both direct and indirect oxidations, which in the first

one, pollutants are absorbed by anode’s surface and then degraded by the reaction of anodic
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electron transfer. Whereas indirect oxidation leads to electrochemically generated strong

oxidants like hypochlorite/chlorine, hydrogen peroxide, and ozone [128]. OH • is a reactive

oxygen species with 2.80 V/SHE standard redox potential (E°) which is electrocatalytically

originated by the following reactions [129], [130]:

28
M + H2 O  → M (OH • ) + H + + e− (1)

R + M (OH • ) → M + CO2 + H2 O (2)

In these reactions, M is the metal surface and R is organic specie.

Active chlorine, in the form of gaseous chlorine, hypochlorite ions or hypochlorous acid, is

anodically produced from chlorides which are naturally present in or added to the solution

[130]:

2 Cl− → Cl2 + 2 e− (3)

Cl2 + H2 O → HOCl + H + + Cl− (4)

HOCl → H + + OCl− (5)

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Although this process is efficient in eliminating of coloring and organic substances, it is not

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economically advantageous nowadays because of the low process stability and considerable

operational cost [29],[131].

-p
4.3. Physical processes for dye removal from wastewater
re
Mass transfer mechanism is the base of the physical dye removal methods [14]. These methods

have 86.8-99% range of dye removal, with the adsorption process ranking highest among all.
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These are capable of degrading almost any dye or a mixture of dyes easily [14]. Physical

methods, as a commonly used method among all three methods (biological, chemical, and
na

physical), are usually straightforward. Different characteristics like cheapness, simple design,

and easy operation, high efficiency, no effect by toxic substances, and low costs have made the
ur

adsorption techniques to be a productive process for treating polluted waters. The low necessity

of chemicals is another advantageous feature of this method [132]. This treatment seems to be
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more predictable than the two other treatments because of its independence of living organisms

[14].

4.3.1. Adsorption

29
This method is considered as a surface phenomenon in which the molecules of adsorbate or

ions (gas or liquid) are attracted to the surface of adsorbent (solid) (Fig. 11). Physisorption or

chemisorption are the two classes of adsorption. These categorizations depend on the way that

dye molecules or other elements get adsorbed onto the adsorbent surface [41]. Different types

of forces may exist in the adsorption process of dye molecules such as hydrogen bonding, van

der wall forces, electrostatic and hydrophobic interactions, etc. [133].

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Fig. 11. Dye adsorption with activated carbon.

Commonly, adsorbents contain porous structure in order to be more efficient in adsorption.

na

This structure increases the total exposed surface area and allows fluid to cross faster. This

method used as a simple and cost-effective technique for removing dyes from wastewater
ur

[134]. High treatment efficiency and being reusable are some of the advantageous features of
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this method. The performance of most of the adsorbents is controlled by different factors which

the main ones are initial dye concentration, pH, temperature, contact time, and adsorbent

amount. Possessing porous structure (resulting in high surface area) and low adsorption

equilibrium established time for removing dye wastes in lesser time, result in a suitable

adsorbent [135],[136].

30
The most determinative element of the adsorption process is the adsorbent. Adsorption

capacity, surface area, short adsorption period are the most important factors of an adsorbent

[52],[137]. Alumina, activated carbon, zeolites, and silica gel are commonly used for the

removal of dye from wastewater [41]. Porous structure with high surface area and great

adsorption capacities towards various kind of pollutants are the factors which have made

activated carbon (AC) well-known [138]. Table 5 depicts a review on the studies furthered on

treatment of dye-containing wastewater by using adsorption in the last two years.

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31
 Table 5. A review on the studies furthered on treatment of dye-containing wastewater by using adsorption in the last two years.

Dye Adsorbent Dye concentration pH Temperature Adsorbent dose Decolorization References

(mg L-1) (K) (g L-1)

Orange G Alumina nanoparticles 19.4 2.5 303 1 63.9% ]311[

Indigo Carmine 64.1%
Reactive Red 180 17.3 56.6%
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24

Methyl Orange Co3O4 nanoparticles 50 6 303 0.05-0.5 %11< ]311[

>%311
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Sunset Yellow Chitosan (Ch)–Vermiculite (V) composite 25-1000 38-3 278, 298, 313 1.11 Quite high [141]
Brilliant Blue beads
10-1000
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Sunset Yellow 0.007 g of polypyrrole/multiwall 30 8 812 1.11-1.1113 ~99% ]318[
carbonnanotubes nanocomposite 1.11-1.1113
Congo Red 0.01 g of polypyrrole/multiwall carbon 30 8 812 ~98%
nanotubes nanocomposite

32
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Methylene Blue The optimized cellulose/montmorillonite 30, 80, 100 4, 6, 7, 9 298, 313, 323 Almost 100% ]311[
(MTM) hydrogels re
Methylene Blue Composite structure of montmorillonites 750 8 111 94.3% ]311[
(Mt) with graphene oxid (GO) (Mt/GO) -p
Congo Red ZnO@Ze composite particles 25–500 3−12 111 0.025– 0.1  Up to 90% ]311[
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Food Red 17 Bio–based polyurethane/chitosan foam 25 8 182 3 >98% ]311[
(PU/chitosan)

Crystal Violet Biopolymer/ZSM–5 zeolite 15 1.1 182 8 75.3% ]311[

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Methylene Blue 15 2 86.6%
Basic Fuchsin 15 1 81.2%
4.3.2. Membrane filtration

One of the cutting-edge treatment technologies for removing color, COD, and salinity from

wastewater is membrane filtration [148],[149]. In this procedure, wastewater passes through

the membrane, which has small pores that makes the solutes bigger than these pores to be

trapped behind it, and then the passed solution is exempt from those solutes. The trapped

solutes create a filter cake layer. In order to have an easy filtration process, these layers must

be continuously cleaned. The pores' size is one of the factors that membranes can be

categorized based on that. Rejection and permeates flux usually defines the membranes'

performance [4].

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4.3.2.1. Microfiltration (MF)

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In this membrane process, contaminants from the fluid are removed by microporous
-p
membranes. A classification of a typical microfiltration membrane can be based on its pore

size range, which is between 0.1 to 10 micrometer (μm). One of the applications of this process
re
is to remove suspended solid particles [150].
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4.3.2.2. Ultrafiltration (UF)

Ultrafiltration membranes with pore sizes between 0.1 to 0.001 microns are more economical
na

because of requiring lower pressure than nanofiltration and reverse osmosis. However, low

rejection is caused by large pore size [150].

ur

Micellar-enhanced ultrafiltration (MEUF) is a practical process for removing organic dyes

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from wastewater. Whereas several researches have presented MEUF as a proper technique for

retention of anions, metal ions, and organic contaminants, but this method has not been used

on an industrial scale. In this method, a surfactant is added to an aqueous solution with

pollutants, which has a higher concentration in comparison with CMC (critical micelle

concentration). As a result, the organic and inorganic contaminants are solved by the formed

micelles of surfactant molecules. Then these micelles which contain the dissolved solutes are

33
rejected at the time of membrane ultrafiltration treatment. After passing a permeate stream

through the membrane, they are almost without pollutants [151].

4.3.2.3. Nanofiltration (NF)

Nanofiltration (NF) is a novel advanced membrane technology that is applicable for diverse

wastewater treatment and decontamination applications [152]. Lately, nanofiltration (NF) has

been proven as a promising separation technology to replace or complement some of the

conventional separation techniques, exclusively in the removal of dyes [153]. These

membranes remove the dyes efficiently because of having charge and the pore size between

of
0.5 to 2.0nm in diameter [152], [154]. Thus, they can effectively reject various dye molecules

via both the size and electrostatic repulsion mechanisms. This technology has depicted features

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between ultrafiltration (UF) and reverse osmosis (RO) [155],[4]. For instance, Kurt et al.

studied on a commercial NF membrane (NF-270, Dow Filmtec, with a molecular weight cutoff
-p
(MWCO) of 200-300) to eliminate colors, COD (chemical oxidation demand) and salts from
re
the weaving industry effluent. Under the continuous mode, the NF-270 was found to eliminate

nearly 100% of the colors, reject up to 94.7% of the COD, and 76.3% of the salts [156]. In
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addition, NF also has lower fouling tendency and lower energy consumption, lower osmotic

pressure difference, higher permeate flux, higher retention of multivalent salts, relatively low
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investment and low operation maintenance costs are the advantages of NF which indicates

more excellence than UF and RO [157], [158], [159].

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4.3.2.4. Reverse osmosis (RO)

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The process of using semi-permeable spiral wound membranes for separating and removing

dissolved solids, organics, submicron colloidal matter, pyrogens, nitrate, bacteria, and color

from water is defined as reverse osmosis (RO) [160]. This process has been used for industrial

applications in the removal of colors and salts from solutions, furnishing an almost deionized

water [161]. Achieving concentration and separation with no state change and no thermal

34
energy or chemicals using are the advantages of this membrane-based process and technology.

These features make efficient process energy and suitable applications for recovery. The

beverage industry, distillery spent wash, groundwater treatment, recovery of phenol

compounds, and reclamation of wastewater and seawater reverse osmosis (SWRO) treatment

are some of the applications of RO systems, which indicate their efficiency[160].

Table 6 depicts a review on the studies furthered on treatment of dye-containing wastewater by

using membrane filtration in the last two years.

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35
 Table 6. A review on the studies furthered on treatment of dye-containing wastewater by using membrane filtration in the last two years.
Pure water Dye
Membrane Pore radius Pressure
Dye permeability concentration Contact angle Decolorization References
(bar)
(mg L-1)

Reactive Green 19 PES-Fe3O4-MDA (0.5 wt%) - NF 7.44 nm 185.7 1 100 37.18° ~98% [162]
(L/m2.h)

Methylene Blue 0.5 wt. % ZnO/cGO nanohybrid in hollow 7.92 nm 358.5 ± 14.9 11 98.6 ± 1.4%
1 35.3±1.1° ]311[
Rhodamine B fiber membranes - NF (L/m2. h mmHg) 8 98.5 ± 1.1%
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Alizarin Yellow PA1/TA 0.08 thin-film nanocomposite 103.2 97.5%
Sunset Yellow membrane 25.3 nm (L/m2h. mPa) 1 311 36.7±1.6° 99.9% ]311[
Congo Red 99.9%
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Congo Red 14.8 
PES/UiO-66 membrane - NF 0.25-0.28 nm (L/m2.h.bar) 2 40 50◦ 99.9% [165]
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Zwitterionic N, N Bis (3-aminopropyl)
10.67
methylamine, ZDNMA (1 wt%) and TMC
Methyl Blue 0.27 nm (L/m2.h.bar) 1 300 30-45° 99.9% [166]
NF

36
lP
Blue Corazol PES/PEI 3.0 + GO 0.025 + PEI 1.5
99.4
(Reactive Black 5 and MF 0.2 μm 1 10 59.3 ± 4° 97.8% [167]
(L/m2.h.bar)
Reactive Blue 220)
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Bright Blue food MF PEI5 GO1 TA4 20.52 79° ± 9° %311
coloring MF PEI5 GO1 TA0 0.2 μm 23.35 1 10 78° ± 3° 88.26% [168]
MF PEI5 GO0 TA4 736.35 57° ± 3° 16.05%
(L/m2.h.bar)
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Two textile dye Ceramic membrane 1376
bath effluents 0.27 μm 3 26% [169]
MF (L/m2.h.bar)

Rhodamine B
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Polyether sulfone (PES) microfiltration 4777
0.1 μm 5 >98.9% [170]
membrane (L/m2.h.bar)

Cellulose nanofibrous membrane

prepared by in-situ synthesis of ZIF-8 in
of
84
Cationic dye TEMPO-oxidized bacterial cellulose 20 μm 1∼3 10 >99% [171]
(L/m2.h.bar)
nanofibers (TOCN) dispersion
(ZIF-8/ TOCN)
 Table 6. continued

Pure water Dye

Membrane Pore radius Pressure Contact
Dye permeability concentration Decolorization References
(bar) angle
(mg L-1)

Methyl Orange Chitosan enhanced cellulose membrane 107. 28 1 0.1 mM 19.50° 86% [172]
Direct Blue 71 UF (L/m2.h.bar) 89%
PPSU/ SnO2 mixed matrix hollow fiber
Reactive Black 5 membranes (HFMs) -UF 362.9  >94%
8 11 63.7 0 ]311[
Reactive Orange 16 (L/m2. h) >73%
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Polyimide (PI) membrane
345.10
Direct Red 23 UF 3 311 67.6° 98.65% ]311[
(L/m2. h)
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Direct Red 80 Ceramic membrane made from purified 14.7 
natural Moroccan clays 75 nm 1 50 99% [175]
(L/m2. h)
UF
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Al3+- doped TiO2 (AT) tight 9.6
Alizarin Red-S 3.5 nm 1 250 19.4° 96.9% [176]
UF (L/m2.h.bar)

37
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27.7
Acid Black 210 PPSU 20%–PES 4% membraneUF 313.31nm 1 35, 45, 65 68.1 ± 1.51° >99.65% [177]
(L/m2. h)
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Polypropylene composite hollow fiber
Congo Red membrane (PPM1.49) 81.8
0.15±0.0 μm 1 50 37 o 99.5% [178]
UF (L/m2. h)
-p
Congo Red PSf/PVA/ZnO (0.5 w.t. %) ~55 53.5%
(J/J0) 3 100 43° [179]
UF

Not specify
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Spiral wound membrane 19 Almost
5 μm ~8 28 [180]
RO (L/m2. h) compeletely

36.39
Methylene Blue
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34.99 100 91.34-100%
Methyl Orange PES/TiO2 halloysite nano-tubes (NTs) 1.149 μm 1.8 45 ± 1.5o [181]
(L/m2. h) 100 68.33-100%
membrane
RO-NF
4.3.3. Ion exchange method

Ion exchange method has absorbed interests vastly. High efficiency, low costs, and attractive

features have made it suitable for applications such as water purification, heavy metals

removal, and textile effluents treatment. Removing dyes by strong interactions between

functional groups on ion exchange resins and charged dyes is one of the effective processes of

this method. In this process, achieving effective separation is caused by forming strong bonds

between resins and solutes [182],[4]. Anion exchangers or cation exchangers as resins are being

used to separate solutes with different surface charges [183]. Table 7 presents some recent

studies on dye removal by ion exchange.

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Table 7. Some recent studies on ion exchange for removal of dyes.

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Dye Anion/cation exchanger Dye removal Dye concentration References

Acid Orange 10 Amberlite IRA 400 anion-

exchange resin
-p
96.8% 10−2 M [184]

Acid Black synthesized cellulose anion almost 100% 300 mg L-1 [185]
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exchanger (CellAE)

Direct Red R (HPMA-coEGDMA-co-GMA)- 89.4% 10-500 mg L-1 [186]

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Disperse Violet 28 SO3H terpolymer resin cation 91.7%

exchanger
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Fig. 12 categorizes the advantages and disadvantages of different technologies used for color

removal from wastewater.

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Fig. 12. A glance of dye removal technologies with their advantages and disadvantages [14],[47].

39
4.4. Hybrid treatments

Recently, researchers have paid heed to hybrid processes. Based on the fact that each dye

removal process has its own advantages and disadvantages, a combination of different

techniques can be used to have efficient dye removal. Mixing up easily and wrong classification

are defined clearly in combined processes and hybrid processes vitally. A combined process is

defined as a process in which two or more treatments are furthered sequentially. A hybrid

process is defined as a process where two or more treatments are fused into one process [187].

In hybrid processes, integrating treatments adjust the individual treatment criteria [188].

Basically, a hybrid process, as a cost-saving and time-saving process, requires one vessel for

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carrying out the multiple processes which are integrated into one [189].

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The next section discusses the perspectives of textile wastewater treatment using MBR and

PMR systems. -p
PMR and MBR: two promising hybrid technologies
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The interrelations between the three major dye removal technologies, PMR and MBR hybrid
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processes are depicted in the Venn diagram in Fig. 13.

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Fig. 13. The interrelations between the three major dye removal technologies, PMR and MBR hybrid

processes.

40
The objective of this part is to overview the progress in the configurations and applications of

these technologies and also, organizes the results and information from studies conducted

recently on the performance of using MBR and PMR technologies for textile wastewater

treatment.

4.4.1. MBR technology

This system was first presented in 1968s as a combined membrane unit [190]. MBR process

has some advantages such as low maintenance, lower sludge production, small footprint,

consistency in final treated water quality independent of sludge conditions in the bioreactor,

of
and higher removal of organic and nutrients pollutants over conventional activated sludge

processes [191]. Furthermore, one of the major advantages of membrane bioreactor treatment

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over more conventional processes in dye removal is its high efficiency in microorganisms'

retention [192]. -p
However, membrane fouling is the main weakness of the MBR process, which is defined as an
re
irreversible deposit of layer materials on the surface of membrane with a possible existence

and growth of microorganisms on it [191],[193]. It results in declining the permeate flux or

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increasing the trans-membrane pressure (TMP) with processing time, causing higher operating

costs for cleaning the membrane and finally decreases the membranes life span
na

[194],[195],[196]. The filtration flow can be improved, and the membrane fouling can be

solved by applying a suitable physical, chemical or biological cleaning to the membrane

ur

[197],[198].
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Whereas this technology is highly costed in set up and it is overcome by the reuse of permeate,

in comparison to other conventional treatment technologies, MBR has resulted in superior

performance and applicable technique for operating the domestic and a full scale of industrial

wastewaters [199],[200].

41
This process consists of different stages, firstly started by feed wastewater as feeding, and then

it comes into the reactor to interact with the biomass. The second stage is pumping the mixture

of feed wastewater and biomass to the membrane unit, and then the retentate is recycled after

discharging the permeate into the separation unit [200],[194]. Membranes with the pore size

range of 10-4 - 10-3 µm are used in MBR systems, and the process could be referred either as

microfiltration (MF) or ultrafiltration (UF).

MBRs often are categorized according to their aeration processes, which is discussed in the

following sections. Another way to categorize MBR systems considered the system setup. To

be exact, the membrane modules could be located in a separate tank (side-stream system) or in

of
the bioreactor tank itself (submerged system) as it is shown in Fig. 14. Regardless of the

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aforementioned configurations, the membrane itself can be in the shape of a hollow fiber or

flat sheet [201]. All of these options are a critical aspect of designing a wastewater treatment
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plant and need to be delicately selected based on certain requirements of the system.
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Fig. 14. Membrane bioreactor configurations based on location of the membrane.

4.4.1.1. Aerobic MBR (AeMBR)

42
Nowadays, this type of MBR as a reputable process is being used for textile wastewater

treatment. It will be used in a situation that COD removal efficiency is more than 90%.

Meanwhile, decolorization from printing and dyeing stages has gained much attention [202].

Using aerobic MBR treatment by Yun et al. resulted in 94.8% COD removal and 72.9% dye

removal. It is known that adsorption to microbial cells followed by sludge withdrawal can only

remove synthetic azo dye which cannot be biodegraded [203]. Hoinkis et al. studied the COD

concentration (600 and 1250 mg L-1) effect on the MBR system. The removal efficiency for

COD, ammonium, and color reported being more than 90%, 90%, and 60-75% consecutively

[204]. An enhanced membrane bioreactor (eMBR) was investigated by Rondon et al. It

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consisted of two anoxic bioreactors afterward, an aerobic membrane bioreactor, a UV

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decontamination unit, and a GAC (granular activated carbon) filter to process a synthetic textile

effluent called Blue Remazol (BR) over 100 days. 95% of BR and 99.1% of COD were
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removed by this system. Whereas, MBR is an efficient treatment for textile wastewaters,

membrane fouling as a significant problem is limiting its application [205].

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4.4.1.2. Anaerobic MBR (AnMBR)
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Anaerobic MBRs used for textile wastewater treatment and have been investigated in several

studies. In those, they show an excellent technology for wastewater treatment. A review study

by Lin et al. showed that food industrial wastewater treatment is the most famous applicable
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industry for AnMBR. Using AnMBR for textile wastewater treatment has been reported once

before the year 2013 [206].

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Production of biogas is a significant advantage of anaerobic MBR. Therefore, as a highly

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required process, advance of active and economic biogas recovery (main methane) is used to

make the anaerobic MBR technology economically possible [199]. Biogas production could

be observed in anaerobic MBR technology during wastewater treatment based on the founding

of several studies. Producing biogas with an excellent fuel quality followed by anaerobic MBRs

43
have been noted by Hu and Stuckey. This study shows that this biogas consists of 80% methane

[207].

Anaerobic MBR system has low energy consumption for mineralizing the organics. Producing

low sludge, low nutrient requirement, cost-effective for wastewater treatment, especially for

those dye textile wastewater and generating useful methane as an end-product are some of the

advantages of anaerobic MBR [199],[208]. Achilli et al. furthered research comparing the

operational cost of an aerobic and anaerobic treatment for urban wastewater treatment. It has

been presented in this study that aerobic MBR had more operational costs in comparison to

anaerobic MBR since aerobic MBR has excess sludge management [209]. The application of

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MBR (anaerobic and aerobic) for the treatment of synthetic textile wastewater were

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investigated by Yurtsever et al. Both MBRs had efficiencies for removing high COD. Whereas

the efficiency of dye elimination was only 30-50% in aerobic MBR, anaerobic MBR showed
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100% dye removal. Whereas the research presented lack of color removal in MBR process and

requiring a post-treatment process to ensure a satisfactory textile wastewater treatment, a

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combination of aerobic and anaerobic MBR process is able to be used for dye removal and
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energy saving [210]. Adopting anaerobic-aerobic processes in the MBR system are making an

economical way for such application [199].

The application of membrane separation for different types of textile wastewater has been
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studied in several investigations. Table 8 depicts a review on the studies furthered on treatment

of textile wastewater by using MBR in the last two years.

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 Table 8. A review on the studies furthered on treatment of textile wastewater by using MBR in the last two years.

MBR Anaerobic BOD COD Dye

Sample Dye Membrane Remarkable results Refrences
configuration or aerobic removal removal removal

3Remazol 3D printed Wastewater was

RBBR and sulfate based
Brilliant Blue R Side-stream dynamic membrane Anaerobic - >93.0% >96.7% pretreated with ozone [208]
synthetic textile wastewater
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(RBBR) module support using ozone machine.

Hollow fiber
Capital and operational
62%
Woolen textile 74% 70% costs were estimated for
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- Submerged MBR Aerobic 80% [211]
wastewater 99% 97% full-scale MBR.
MBR+NF 85%
99% 99%
MBR+RO
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UF Study of the effect of
Al-Kut textile factory HRT and MLSS on the
- Submerged Aerobic - [212]
wastewater MBR 88.34% 83.7% removal efficiency by
MBR+RO 99.8% 99.8% MBR.

45
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Suggested that the
osmotic membrane
Synthetic dyeing Lanaset Red Osmotic bioreactor (OMBR)
Submerged Anaerobic - ~99.4% ~100% [213]
wastewater G.GR (Acid dye) membrane
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for treatment of dyeing
wastewater.
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Dead-end
Simulated printing and Methyl filtration
Submerged Anaerobic - - 100% [214]
dying wastewater Orange (PVDF flat
sheet membrane)
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Simulated textile Diamozol Red Submerged UF Aerobic - 79% 76% [215]
wastewater ED-3
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4.4.2 PMR technology

Smaller dye molecules resulted by breaking the large ones is one of the potentials of PMR

technology because of the photocatalyst’s action, which mainly water and carbon dioxide are

produced at last [216]. In a photocatalytic system, photocatalysts are excited by high-energy

photons, which followed by electrons transfer to the conduction band and formed electron-hole

pairs. Reaction of electrons and holes with the oxygen and hydroxyl groups in water is the next

step, which generates various reactive oxygen species like OH, O2− , H2 O2 . Degrading various

types of refractory organic contaminants and strong oxidizing properties are some of the

features of this technique [217]. The mechanism has shown in Fig. 15. Separation of

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photocatalysts from the treated water, good permeate fluxes, antifouling properties, energy-

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saving, and reducing the installation size due to the supplementary operations, are some of the

advantages of PMRs in comparison to conventional photoreactors. It is essential to remove the

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photocatalysts from the processed solution to enhance the effluent purity in a photocatalytic
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reactor. For this mean, coagulation-flocculation-sedimentation are performed

[218],[217],[219].
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Fig. 15. Schematic representation of the activity of photocatalytic membrane and TiO2@HNTs

photocatalyst [220].

In order to have a good performance of photocatalytic membrane reactors, for finalizing to

productive applications, selection of the appropriate process parameters is crucial.

46
Photocatalysts (structures and properties, concentration, type, and loading), membrane (type,

material and pore size of the membrane, and configuration of membrane module), light

(wavelength, intensity, and type of light, the position of the light source), temperature, pressure,

and pH are some of the most important efficient factors of PMR. More details can be found in

[221],[217]. Significant effects on photocatalytic efficiency are caused by band-gap energy,

particle size distribution, crystal composition, porosity, and surface area, as the properties and

structures of photocatalysts. Selecting photocatalysts is highly influenced by band-gap energy

as the most important factor. The most used photocatalyst in PMR is TiO2-based photocatalyst,

because of its distinctive characterization like desirable chemical stability and activity, cost-

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effective, and nontoxicity [222],[217].

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PMRs can be classified into two configurations: the first one is PMRs with suspended

photocatalyst (which is known as slurry reactor) and PMRs with immobilized photocatalyst
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on/in the membrane. Due to the greater active photocatalyst surface area, UV light avoids
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membrane damage and generates hydroxyl radicals in the suspended system in comparison to

the immobilized system. The researchers paid more attention to the PMRs with suspended
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photocatalysts as high-efficient ones [223],[224]. In addition to this classification, the slurry

system can be categorized into two groups: external and internal type. Whereas in the second
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one, the membrane separation process and photocatalytic reaction are fused into one system,

in the first one, two processes occur in separate apparatuses [217],[225]. Cross-flow and dead-
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end are two various operation ways of photocatalytic membrane reactors with an immobilized

photocatalyst. Another classification of photocatalytic membrane reactors is based on the light

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source position, that can be: inside or above the feed container, inside or above the membrane

unit, and in a specific vessel positioned between the membrane unit and the feed container

[221]. All these classifications are shown in Fig. 16 to present more accurate view of PMRs

systems.

47
 of
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Fig. 16. Different configurations of photocatalytic membrane reactors [226],[217].

4.4.2.1. Immobilized photocatalyst

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The immobilized photocatalyst on/in the membrane in PMR leads to a photocatalytic

membrane (PM). Membranes in this system act as a selective barrier for the pollutants that
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should be removed as well as the membrane separation process that furthered in the same unit.

Supports are handled either by using polymeric and ceramic membranes or various organic and
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inorganic materials [227]. Some of the typical polymeric membranes are PA (polyamide),

PVDF (polyvinylidene fluoride), PES (polyethersulfone), PU (polyurethane), PET

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(polyethylene terephthalate), PAN (polyacrylonitrile), PTFE (polytetrafluoroethylene), and CA

(cellulose acetate) [227],[217].

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Different factors control membrane preparation techniques and conditions like membrane

material and the desired structure and morphology. There are different techniques that are being

used for catalytic membrane preparation which the most used and versatile technique for

polymeric membranes is phase inversion [227].

48
A research furthered by Dhananjeyan et al. states that by using immobilized photocatalysis on

TiO2 and Fe2O3 on modified copolymer films, chlorocarbons, and Orange II dye can be

degraded. This study indicates that different factors like the type of scavenger used for

separation of the charges on the semiconductor surface and the organic compound, the physical

characteristics of the bound semiconductor, and the light source control the degradation of

Orange II [228]. A photocatalytic membrane supported on a porous ceramic tube in which

solutes permeation through the membrane and photocatalytic reaction occur simultaneously

has been investigated by Wang et al. Using Acid Red 4 (AR4) dye as a model pollutant led to

following results. Firstly, the decomposition ratios of dead-end and system were five and three

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times higher than the system containing flow rates of 4×10-7 m3 s-1 and 6.67×10-8 m3 s-1,

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respectively. Secondly, increasing irradiation intensity and the amount of loaded catalyst

increases the decomposition ratio, but at higher catalyst loading remain constant. Thirdly,
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increasing flow rates decreases the decomposition ratio [229]. A pluronic-based TiO2 hybrid

photocatalytic membrane was fabricated by Goei et al. with hierarchical porosity using the
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acid-catalyzed sol-gel method. They evaluated the membrane performance in continuous flow
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photoreactor and batched photoreactor in dead-end mode operation. Batch photoreactor could

degrade 100% of Rhodamine B in spite of the limit of mass transfer. A flux with 116 L.m2 h-1

bar water permeability and 3.1×1012 m−1 intrinsic membrane resistance was shown after using
na

the stratified porous Plu A membrane (that is coated with three diverse layers of TiO2 with

diverse pore structures). Finally, a considerable amount of RhB (2700 mg m-2) was removed
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[230]. A hybrid ultrafiltration/photocatalysis method used for elimination or decreasing the

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amount of synthetic dyes in wastewater was investigated by Athanasekou et al. A water

purification system was used for the photocatalytic filtration experiments in continuous flow

conditions. In this study, Methylene Blue and Methyl Orange were used as azo-dyes model

contaminants, under near-UV/vis and visible light irradiation. By examining the consequence

of some factors such as surface area and charge of the photocatalysts, porosity, and amount of

49
that, which are related to both of the hybrid ultrafiltration/photocatalytic method and the

membrane structure, membrane efficiency tried to be optimized. The type of contaminant and

pH of the under-treatment steam were two of the main controllers [156]. The degradation of

Reactive Orange 16 and Reactive Red 180 (azo dye solutions) were studied by Yatmaz et al.

These solutions used in an innovative hybrid process of photocatalytic membrane distillation

(MD) process in textile industry wastewater. Hir et al. used phase inversion technique for

preparation of a series of PES/TiO2 (polyethersulfone-TiO2) film photocatalyst using for

Methyl Orange photodegradation. By increasing films photoactivity, an increase in TiO2

content up to 13 wt% (PT-13) took place. In this study Methyl Orange was almost completely

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removed in acidic conditions. Methyl Orange photodegradation followed pseudo first-order

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kinetics and the PT-13 film showed to be efficient to gain a high degradation even after five

cycles which shows the stability of the film photocatalyst [231].

4.4.2.2. Suspended photocatalyst

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This process contains the dispersion of photocatalyst in the feed solution evenly, and in order

to recover the photocatalyst from the treated solution, a membrane can be used independently.
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This technique has some advantages, including being in contact with the pollutants sufficiently

as a noteworthy advantage that is due to the higher surface area. Besides, whereas increasing
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of photocatalyst dosage is not possible for the immobilized system due to the inadequate

membrane surface area, it is feasible to increase in a wide-ranging suspended system. All in

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all, higher productivity and more capable for applications in large-scale industries are the

features of PMR [232],[217]. As a salient example among several reports on using this
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configuration for dye removal and purification, Congo Red (C32H22N6Na2O6S2) and Patent

Blue (C27H31N2NaO6S2) were degraded in aqueous solution by Molinari et al. This process

furthered in a photocatalytic membrane reactor using TiO2 Degussa P25 as the catalyst. Congo

Red was depicted to be photodegraded faster in the same experimental situation; it could be

because of the higher absorption on the catalyst surface. As an interesting note, this treatment

50
is successful in being used in solutions with high concentration (500 mg L-1) of both mentioned

dyes which furthers in a continuous process reaching adequate fluxes of permeate (30-70

L m-2 h-1). The reactor containing the suspended photocatalyst performed more efficiently in

comparison to the PMR with immobilized catalyst [233]. This type of PMR technology for

decolorization means was investigated by Damodar et al. The material used for membrane in

this study was polytetrafluoroethylene (PTFE), which the pore size of it was 0.22 mm and the

contact angle value was 120°. The removal of color (100%) in a high-performance state and

80% removal of TOC and COD was the result of this study. Photocatalyst in PMR was reported

not only to have the ability to be reused and be separated effectively but also to be able to keep

of
its activity for long-term use. During continuous filtration operation, the distribution of TiO2

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particle size presented a momentous diversity. This study also indicates the benefits of their

operating conditions to have a longer operation and reducing the regular requirement for
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cleaning the membrane [234]. The consequence of presenting ZnO nanoparticles in PMR for

removing Congo Red (CR) was studied by Hairom et al. The membrane used for this study
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was polypiperazine amide, which is a nanofiltration (NF) membrane. Under active stirring
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(represented ZnO-PVP-St), synthetic nanoparticles with polyvinylpyrrolidone showed the

highest photodegradation efficiency. Furthermore, they showed the lowest effect on the
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membrane flux decline from all the ZnO samples tested. The results of this study indicated that

0.3 g L-1 optimum loading for photocatalyst was achieved with 20 mg L-1 initial dye

concentration at pH 7, which the effective surface area of ZnO-PVP-St and the presence of UV
ur

light are the terms explaining it [235]. Yatmaz et al. scrutinized the degradation of Reactive
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Orange 16 and Reactive Red 180 (azo dye solutions) from the wastewater of the textile

industry. In this study, an innovative hybrid photocatalytic and membrane distillation process

was used. These two processes used as sequencing and hybrid system. The stages of this

technique consist of: 1) studying the photocatalytic process to determine the optimum

conditions and the best efficiency in which the highest amount of COD and color removal were

51
obtained using the ZnO catalyst (1 g L-1) and UVA light for RR 180 dye in photocatalytic

process. 2) connection of the membrane distillation unit to the photocatalytic reactor for

furthering the treatment, which in this case, increasing flow rates (from 210 to 665 mL min-1),

led to increasing the amount of collected distillate. As a result, easing the operation while

maintaining a small footprint was obtained as membrane distillation was used to separate the

catalyst particles provided. Finally, the color removal efficiency improved up to 100% for both

dye solutions as the membrane distillation unit integrated after the photocatalysis process [236].

A summary of the researches on treatment of textile wastewater by using PMR in the last two

years is shown in Table 9.

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 Table 9. A review on the studies furthered on treatment of textile wastewater by using PMR in the last two years.

Sample Dye PMR configuration Photocatalyst Membrane Irradiation COD removal Dye removal References

A mixture solution: Methyl Blue Immobilized P-doped Al2O3 Visible light - > 90% [237]
MB (5 ppm), MO g-C3N4 (PCN) hollow fiber
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(8.1 ppm), and phenol
(3.3 ppm)

Palm oil mill - Suspended ZnO−CC Nanofiltrati UV 99.97% 99.84% [238]

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secondary effluent on (NF-TS 40)
(POMSE)
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Textile factory - Suspended -external ZnO-PEG Ultrafiltrati UV Lower ~100% [239]
wastewater (SDWW) on (UF-PPA) compared to the
original SDWW

53
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Bulk solution of Methyl Blue Immobilized – PDA/ZIF-67 Flat sheet Visible light 92.3% [240]
MB and MO Methyl Orange cross flow polypropylene -
(PP) membrane 99.5%
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Eosin Yellow Immobilized N, Pd co-doped PSf Visible light - 97% [241]
TiO2 polymeric
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membrane

Reactive Black 5 Immobilized Fe3+@ ZnO polyester Solar - 98.34% [242]

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membrane radiation
fabric
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Recently a study has evaluated the performance efficiency of integrated MBR systems with

photocatalysis to process a sample of real textile wastewater. Sathya et al. (2019) have

developed a novel MBR (submerged configuration) integrated with ozonation and

photocatalysis and also investigated the membrane fouling phenomena. Through this combined

system, they achieved 94%, 93%, and 100% removal of color, organic, and TSS (total

suspended solids), respectively. It can be concluded from this work, that the combination of

membrane bioreactor and photocatalysis presents an efficient technique to remove organic and

color from textile wastewater [243].

To conclude the PMR section, the photocatalytic performance of some nanoparticles is going

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to be discussed, which is one of the most critical factors in this system's efficiency.

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The photocatalytic performance of nanoparticles has been attracting considerable attention for

dye removal applications in recent years as a cost-effective and green method [244],[245].
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Metal oxide semiconductors are promising candidates as photocatalytic nanoparticles for
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degradation of organic pollutants and water purification [246],[247]. Among numerous metal

oxides, ZnO (zinc oxide) nanomaterials are critically important as a n-type semiconductor,
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which have been thoroughly studied in a recent decade because of its exceptional properties

such as high photosensitivity, high electron mobility, biocompatibility, chemical stability, and
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nontoxicity [248]. Decreasing the particle size consequences in reinforced specific surface area,

and the higher number of active sites while repressing recombination of electron-hole pairs
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[249],[250]. The presence of defects, steps, kinks, and sharp edges on exposed surfaces

eventually outcomes in higher surface energy to facilitate photocatalytic dye degrading [251].
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The application of nanoparticles for degradation or removal of textile dyes in some recent

researches is presented in Table 10. The data are reported in recent researches in order to show

the most efficient nanoparticles for certain abovementioned applications. As shown in the table,

the photocatalytic process is the major process for the utilization of nanoparticles for

degradation or removal of dyes from textile wastewater. In general, the degradation of dyes

54
using this method could reach high removal performance from 90 to 100%, under equitable

duration (below 300 min). The remarkable property of the photocatalytic degradation of dyes

in the reports is the dominance of the efforts to represent the potential of visible light,

specifically sunlight. The advanced nanomaterials or composites could degrade some

problematic dyes such as Crystal Violet and Rhodamine B and also some popular dyes such as

Congo Red, Methylene Blue, and Methyl Orange. From the perspective of the nanomaterials,

there are several forms of nanoparticles for the degradation or removal of textile dyes, i.e. (a)

powder (single-core, with or without doping), (b) decorated (core nanoparticles covered with

smaller particles), (c) composite (core nanoparticles were embedded onto a surface larger than

of
the nanoparticles) [252].

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55
 Table 10. A review on recent studies on treatment of textile wastewater by using photocatalytic nanoparticles in the last two years.

Nanoparticle Core material Surrounding material Dye Dye removal Irradiation Removal time References
type (min)

Composite Au/ ZnO/ reduced Methylene Blue >95% Sunlight 30 [253]

graphene oxide
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Powder Titania nanotubes Rhodamine B 91% Sunlight 180 [254]
Methyl Orange 87% 180

Decorated Graphene nanosheets Biphasic TiO2 Methylene Blue 93–98 % Sunlight 60 [255]
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Congo Red 93-98 % 60

Decorated Flower-like NiAl-layered Black Cu-doped Methyl Orange >95% Visible light 60 [256]
double hydroxide TiO2 nanoparticles
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microspheres

Composite Zn/Ti-layered Ag-layered Rhodamine B >90% Visible light 60 [257]

double hydroxide Double hydroxide

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Composite Au@Ag@AgCl Malachite Green 98% Sunlight 110 [258]
Oxalate (MGO)

Composite ZnFe2O4/Graphene Congo Red 92.21% Sunlight 270 [259]

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NiFe2O4 Irgalite Violet 99% Sunlight 60 [260]
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Composite Pt-doped Titanate Methylene Blue 93.5% UV 120 [261]
nanomaterials Rhodamine B 93.9%

Composite TiO2/ZnO/rGO Methylene Blue

ro 99.6% Visible light 180 [262]
and UV

Composite AgIO4/ZnO Rhodamine B 81% Sunlight 180 [263]

Indigo Carmine 98% and UV
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Composite Ag3PO4/TiO2/SiO2 Methylene Blue 99% Sunlight 15 [264]
Conclusions

A wide range of physical, chemical and biological technologies for the removal of dyes from

wastewater were reviewed. Evidently, each of these technologies has its own advantages and

drawbacks. By using a hybrid packing materials and integrated processes, very high color

removal can be achieved and mixture of dyes can be treated. MBR and PMR technologies are

simple, reliable and cost-effective processes that have been investigated for the treatment of

textile wastewater. However, a major drawback in implementing these technologies at the

commercial scale is membrane fouling which reduces the permeate flux and therefore,

membrane cleaning is required. Thus, for long-term reliability of these technologies, the

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operational conditions should be optimized at the lab and pilot-scales and life cycle impact

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analysis and cost-benefit analysis studies should be carried out to demonstrate the effectiveness

of hybrid technologies at the industrial scale.

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Declaration of interests
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The authors declare that they have no known competing financial interests or personal
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relationships that could have appeared to influence the work reported in this paper.
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Acknowledgements
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The authors gratefully acknowledge the assistance offered by the UNESCO Chair on Water

Reuse in Iran. The authors would like to thank IHE Delft (The Netherlands) for providing

infrastructural and staff time support (“Support to the Society”) to collaborate with researchers

from Iran on topics related to water, wastewater, and resource recovery.

57
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