Investigation of segregated wastewater streams reusability with membrane process for textile industry

Accepted Manuscript Investigation of segregated wastewater streams reusability with membrane process for textile industry Kashif Nadeem, Gokce Tezcanlı Guyer, Bulent Keskinler, Nadir Dizge PII:

S0959-6526(19)31292-2

DOI:

https://doi.org/10.1016/j.jclepro.2019.04.205

Reference:

JCLP 16561

To appear in:

Journal of Cleaner Production

Received Date: 19 November 2018 Revised Date:

16 April 2019

Accepted Date: 17 April 2019

Please cite this article as: Nadeem K, Guyer GokceTezcanlı, Keskinler B, Dizge N, Investigation of segregated wastewater streams reusability with membrane process for textile industry, Journal of Cleaner Production (2019), doi: https://doi.org/10.1016/j.jclepro.2019.04.205. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

ACCEPTED MANUSCRIPT

Investigation of segregated wastewater streams

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industry

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reusability with membrane process for textile

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Resubmitted to: Journal of Cleaner Production 16/04/2019

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Institute National Polytechnic - ENSIACET, Toulouse, France

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Kashif Nadeem 1, Gokce Tezcanlı Guyer 2*, Bulent Keskinler 4, Nadir Dizge 3**

Tevfikpasa St, Ozgul Apt, 21/8, 34726, Kalamıs, Istanbul, Turkey

Mersin University, Department of Environmental Engineering, 33343 Yenisehir, Mersin, Turkey

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Gebze Technical University, Department of Environmental Engineering, 41400 Gebze, Kocaeli,

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Turkey

corresponding authors

E-mail: * [email protected]; ** [email protected]

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ACCEPTED MANUSCRIPT Abstract The reuse and recycling of water in an industry is a hot topic in today's growing economy; considering water scarcity, strict regulations for discharge and the high cost of water treatment and supply. This study was planned to investigate the treatment and recycling potential of textile wastewater using membrane technology. Several combinations of ultrafiltration (UF) and

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nanofiltration (NF) membranes were applied both independently and in sequential arrangements to find the most suitable option for each type of segregated wastewater flow. However, dyeing and first washing wastewater with high salinity, the configuration of UP005+NF200+NF90 in a sequential arrangement provided 99.4% color, 99.1% COD, and 43.2% conductivity rejection. The UF+NF configuration was evaluated as the most promising solution to achieve the required water quality for

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water reuse applications without affecting fabric dyeing parameters and quality in case of pre-

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treatment and post dyeing operations.

Keywords: Textile industry wastewater, water recycling, UF/NF membrane, water quality, fabric

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dyeing.

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1. Introduction Textile wet processing industry, which is one of the highly water and chemicals intensive industries in the world, includes dyeing, finishing, and printing process (Sandin and Peters, 2018) . Utilization of more than 3,600 dyes and 8,000 different chemicals were reported in the literature (Kant,

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2012)(Hussain and Wahab, 2018). Textile wet processing generates wastewater with large amount of spent dyes and chemicals which may have negative impacts on aquatic environment and life (Arora, 2014)(Holkar et al., 2016a) (Madhav et al., 2018). As per the estimates available from literature, approaximately 280,000 tons of textile dyes are discharged annually across the globe and they require extensive treatment processes (Asghar et al., 2015). It has been reported that around 100-200 L of

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freshwater is requred to process 1 kg of the textile product depending on the type of process (Francis and Sosamony, 2016)(Güyer et al., 2016)(Hussain and Wahab, 2018).

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Despite the wastewater production, availability of the freshwater is also a serious concern especially in those countries which are facing water scarcity problem or close to hit water shortages in near future (Negro et al., 2018). Moreover, increasing taxation and stringent limits on ground water abstraction has further worsened the situation (Vajnhandl and Valh, 2014). It is reported that the industrial water consumption is expected to be increased by 50% till 2034 globally, and Turkish textile industry will be facing a severe challenge of water supply (Alkaya and

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Demirer, 2014). Multiple approaches including process intensification, segregation of least polluted waste streams and recycling, biological and phyio-chemical treatment options including coagulationflocculation, adsorption, advanced oxidation processes, and membrane technologies have been successfully applied for treatment of textile wastewater (Nawaz and Ahsan, 2014)(Hayat et al.,

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2015)(Holkar et al., 2016b).

Membrane systems have gained high acceptance in both pollution prevention and water recycling

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in urban and industrial reuse concepts (Warsinger et al., 2018). Membrane treatment systems are helping industries for closing the water loop, reducing fresh water intake and consequently reducing the water pollution. Membrane systems are successfully used for the recovery of precious material like caustic soda, slats, polyvinyl alcohol (PVA), Indigo dyes and other chemicals, leading to cost optimization and pollution control simultaneously and closing the water circuits (Lin et al., 2016). In textile wet processing, there are different wastewater streams, each having its own characteristics. Some of them are highly concentrated like pre-treatment and dye bath effluents whereas stream from rinsing, washing, machine cleaning, bleaching, and finishing are less polluted and could be termed as concentrated streams. It was reported that approximately 60-90% of the process water was used for rinsing/washing which could be easily treated and recycled back into the process (Vajnhandl and Valh, 2014). 3

ACCEPTED MANUSCRIPT The fundamental objective of this study was to treat the segregated wastewater streams such as pretreatment, dyeing and first washing, and post washing wastewater with UP005, NF200, and NF90 membranes in stand alone as well as in sequential modes. Dead-end filtration system was used and permeate quality was monitored measuring of pH, conductivity, color, turbidity, total suspended solids (TSS), total dissolved solids (TDS), and chemical oxygen demand (COD). Moreover, lab scale dyeing procedure was also carried out using membrane permeate and compared with water to be used by

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factory. Other aims were to explore the possibilities for the best treatment scenario and reusing of the membrane effluent to decrease the fresh water requirements, to prevent wastewater formation, to save

also estimated for the best treatment scenario.

2. Materials and Methods

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2.1. Characterization of selected wastewater samples

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energy, and to decrease taxation costs. Moreover, capital, operational, and maintenance costs were

This study was specifically designed for a textile industry located in Çorlu-Turkey, with an average production capacity of 35 tons/day and water consumption of 3,000 m3/day depending upon the fabric material and quality requirments (Güyer et al., 2016)(Nadeem et al., 2017). The problematic area in wet processing industry were identified after scrupulous testing of wastewater for different parameters like pH, conductivity, color, turbidity, TSS, and COD. Depending on the quality and quantity of the

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wastewater; streams were categorized as stream A) pre-treatment wastewater, stream B) dyeing and first washing wastewater, and stream C) post washing wastewater. The detailed explanation of the streams was given in Supplementary Information (Fig. S1). Characteristics of wastewater from the selected batch of cotton dyeing are given in Table 1. It can be clearly seen that conductivity, color,

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TDS, and COD are high and they have to be reduced to meet the reuse limits in the textile industry.

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Table 1. Sample characterization of cotton dyeing wastewater streams Reuse criteria

Pre-treatment

Dyeing and first

Post washing

(stream A)

washing (stream B)

(stream C)

Color (Pt-Co)

370

7,556

2,880

0-20

pH

10.7

10.2

8.1

6.0-8.0

80

1,208

440

500

Parameter

TSS (mg/L)

(Alcaina-Miranda et al., 2009)

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17.1

85.4

38.6

15 (mg/L)

Conductivity

4,873

103,300

3,400

1000

4,150

1,546

559

8-40

COD (mg/L)

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(µS/cm)

2.2. Membrane specifications

Commercially available membranes were used in the filtration experiments. A summary of the

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important specifications of the membranes is given in Table 2. Prior to use, the membranes were stored in distilled water overnight and the NF membranes were compacted under a pressure of 30 bar

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for 1 h.

Table 2. Specifications of the membrane used in the filtration experiments Membrane

pH

Temperature o

Membrane

Supplier

range

( C) (max)

material

UP005

5,000

1-14

95

Polyethersulfone

Microdyn Nadir

NF200

~200-400

NF90

~200-400

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(Da)

3-10

45

Polyamide

Dow Filmtec

2-11

45

Polyamide

Dow Filmtec

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type

Pore size

2.3. Analytical measurements

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For the characterization of raw wastewater and treated effluents, following parameters were monitored using standard analytical methods. Two replicates were performed for all analyses. pH & Conductivity measurements: The pH and conductivity were measured with a multi meter (WTW Multi 340i) with accuracy of ± 0.01 for pH and ±1% for conductivity. Color measurement: Measurement of color was performed according to the single-wavelength method using the Hach DR5000 UV-vis Laboratory Spectrophotometer. The color intensity was determined at three wavelengths: 436, 525, and 620 nm and expressed as absorbance. The wastewater samples were filtered with a 0.45 µm pore size filter paper before color measurements. Turbidity measurement: Turbidity was measured by Hach DR5000 UV-vis Laboratory Spectrophotometer at a wavelength of 520 nm and expressed in Formazine Attenuation Unit (FAU). 5

ACCEPTED MANUSCRIPT TDS & TSS measurements: The procedure was determined by the Standard Methods 2540 C for TDS and 2540 D for TSS (American Public Health Association (APHA), 1999). COD measurement: COD was measured by closed reflux titrimetric method (Standard Method 5220, oxidation with potassium dichromate/sulfuric acid/silver sulfate at 150 oC, accuracy ±3%) (American

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Public Health Association (APHA), 1999).

2.4. Filtration experimental set-up

Filtration experiments were performed in a stainless-steel cylindrical stirred batch cell, dead end filtration module (Sterlitech HP4750 Stirred Cell). This module can be used up to 69 bar pressure for

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circular flat sheet membranes with a diameter of 4.3 cm and an effective filtration area of 0.00146 m2. The volume of the cell was 250 mL. The required pressure was applied by a pressurized cylinder (inert gas normally N2) placed alongside the cell. The applied pressure was varied from 5 to 25 bar

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depending upon the composition of the wastewater stream and membrane. During the experiments, permeate flow as a function of time was monitored by weighing at 1 min intervals (monitoring by a Computer software named RSCom® and permeate samples were taken after a specified period of time). The raw wastewater was filtered using a coarse filter to remove suspended solids before it was used for the filtration experiments. Permeate flux (Jw) values, which represent the volumetric rate of

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flow through the unit membrane area, were calculated according to Eq. (1),

Jw =

V A× t

(1)

where V is the permeate volume (L), A is the surface area of the membrane (m2) and t is the time (h).

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Rejection values (%) of color, COD, and conductivity were calculated according to Eq. (2):

 Cp R (%) = 1 −  Ci

  ×100 

(2)

where R is rejection (%), Cp (mg/L) and Ci (mg/L) represent the solution concentrations in the permeate and in the initial feed solution, respectively.

2.5. Lab scale dyeing procedure It was necessary to investigate the impacts of recovered water on the quality of dyeing process in comparison with the reverse osmosis (RO) treated water (normally used in the wet dyeing laboratory of the selected facility). The criteria used for this assessment are as follows: color variation from the standard color and color fastness for rubbing and washing. Testing has been performed according to

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ACCEPTED MANUSCRIPT the standard of German Institute for Standardization, (DIN 5033). Key steps involved in dyeing with reclaimed water as follows: a) After treating effluents from different wastewater streams, pH was adjusted in the range of 6.5─7.0. b) Different recipes were selected for dyeing of the identical cotton samples with different colors in

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order to make sure that the changing of the color did not have any effect on recycled water analysis.

c) Recipe selected was the same for standard water (RO treated ground water) and reclaimed water for all samples.

d) Reactive dyeing with exhaust method was used at elevated temperature i.e.90 oC for 2.5─3 h.

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Dyes, salts, partial alkalis, and other auxiliaries were added to the dye bath at 25±1 °C. Dye bath was heated to 60 oC for 60 min and then the rest alkali was added and kept running the process for the next 90 min.

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e) Washed off the samples with normal ground water and let them dry in oven for 5 min at 100 oC. f) Analyzed the color variation between the samples through comparing them with standard RO treated ground water using spectrophotometer (HiTech, Data Color, 600)

Spectrophotometer directly gives the final result of the ∆E report which determines whether the sample is yellower, redder, bluer, greener, and the depth of value, chroma, hue of labdip. ∆E value can

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change from 0─100; however, acceptable ∆E value for textile is 1.00. If ∆E value is found ≤1, it means that not visible by human eyes. ∆E value is found between 1─2, it means that visible through very close observation by standard observer.

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3. Results and Discussion

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3.1. Membrane filtration for pre-treatment wastewater (Stream A) Pre-treatment process is used to remove chemicals applied in weaving process including PVA, natural starches, and other finishing agents. Large quantiy of fresh water is required for de-sizing due to the low solubility of PVA (Zhao et al., 2015).

3.1.1. Direct ultrafiltration and nanofiltration UP005 was randomly selected for treatment of stream A wastewater. The experiment was run with a feed volume of 200 mL for 85% recovery at 25±1 °C and at 5 bar transmembrane pressure (TMP). After 1 h filtration experiment, the sample was taken for analytical measurements and flux was calculated with online mass measurement software. The results of analytical measurements are presented in Table 3. It could be seen that 99.9% TSS, 92.3% turbidity, 85.1% color (at 436 nm), 7

ACCEPTED MANUSCRIPT 59.9% COD, and 30.2% conductivity rejection was obtained by UP005 membrane filtration. Permeate was used for fabric dyeing and ∆E value was found >1, resulting in strong discouragment for recycling. The experimental conditions for NF200 membrane were kept the same as UF experiment except of TMP which was adjusted to 25 bar. Table 3 depicted that COD, color, and conductivity rejection

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slightly improved to 94.3%, 97.7% (at 436 nm), and 58.5%, respectively. Moreover, when permeate was tried for fabric dyeing at lab scale, it was found that the quality of the reclaimed water obtained from NF200 membrane did not meet the required color variation limit (∆E≤1). However, it was good enough to use for dyeing dark shades and washing/rinsing operation as the ∆E was found within acceptable limits for the dark shades.

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In order to further improve the quality of reclaimed water, NF90 membrane was used with the same experimental conditions as NF200 membrane. NF90 membrane was run for 50% recovery at

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25±1 °C and it ensured 96.0% COD and 95.9% conductivity rejection at 25 bar. The last column of the Table 3 shows the required water quality for reuse application in textile wet processing. When permeate was used for light shade fabric dyeing, ∆E was found < 1.00. Color and conductivity values of the reclaimed water confirmed to the required reclaimed water specifications; however, COD and pH values were still high and might be a problem for continuous recycling which required for further investigations.

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The water quality requirements for each textile are different. Generally, softened water is required for scouring, dyeing, and printing pastes preparation, but it is not necessary for all the washing cycles. The critical parameters are turbidity (0–15 NTU) and hardness (50–60 mg/L) for reclaimed water (Giwa, 2014). Furthermore, high amounts of other constituents such as heavy metals are not permitted

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in the reclaimed water (Rahman et al., 2016). The use of reclaimed water using various treatment methods in the textile dyeing processes were studied by various researchers and they found that it was possible to use reclaimed water for textile dyeing processes (Varadarajan and Venkatachalam,

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2016)(Starling et al., 2017).

Table 3. Analytical results of direct UP005, NF200, and NF90 membrane filtration for stream A Parameter pH TSS (mg/L) Turbidity (FAU)

Influent

UP005 permeate

NF200 permeate

NF90 permeate

10.7

10.7

10.3

9.7

80

0.08

0.0

0.0

17.1

1.3

0.7

0.1

8

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3,400

2,020

200

COD (mg/L)

4,150

1,664

236

166

436 nm (abs)

0.436

0.065

0.010

0.008

525 nm (abs)

0.161

0.014

0.004

0.001

620 nm (abs)

0.053

0.005

0.002

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Conductivity (µS/cm)

0.001

Flux behavior for different membranes are presented in Fig. 1. The flux for UP005 was gradually

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declining from 22.6 to 12.3 L/m2 h (LMH). The flux declined from 86.7 to 17.3 LMH for NF200 and from 18.5 to 8.2 LMH for NF90 after 1 h. When compared the performance of UP005, NF200, and NF90 membranes in terms of flux and permeate quality, it could be seen that flux performance of

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NF200 was much better than UP005 and NF90. However, maximum color, turbidity, conductivity, TSS, and COD can be removed through NF90 membrane but lower flux can increase the operation cost.

90

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80

60 50 40

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Flux (L/m2 h)

70

UP005 NF200 NF90

30

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20 10

0

0

5 10 15 20 25 30 35 40 45 50 55 60

Time (min)

Fig. 1. Flux behavior of UP005, NF200, and NF90 membranes for stream A

3.1.2. Sequential membrane filtration UP005 membrane was used as pre-treatment step to improve the flux performance of NF90 membrane (Fig. 2). The UF effluent might contain lower molecular weight contaminants than 5,000

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with NF controlled membrane fouling and improved the permeate flux.

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Fig. 2. Sequential membrane filtration (UP005+NF90) for stream A

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The values of COD, conductivity, color and other parameters are summarized in Table 4 for sequential membrane filtration. As it could be seen in the last column of Table 1, the characteristics of reclaimed water were below set limits for recycling, except pH which could be handled through neutralization. To use sequential membrane permeate (UP005+NF90) in dyeing process was conclusive and encouraging for the reuse of NF treated water for technological purposes. UF/NF combination improved COD, color, and conductivity rejection to 99.7%, 99.3%, and

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95.5%, respectively. ∆E was found as 0.813, which was within the acceptable limit for reuse, and this strongly encourged reuse application of treated effluent in all textile wet processing process. It can be

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concluded that using UF as pre-treatment before NF process improved the quality of stream A.

Table 4. Analytical results of sequential membrane filtration (UP005+NF90) for stream A Influent

UP005 permeate

NF90 permeate

10.7

10.7

9.6

80

0.08

0.0

Turbidity (FAU)

17.1

1.3

0.0

Conductivity (µS/cm)

4,873

3,400

220

COD (mg/L)

4,150

1,664

14

436 nm (abs)

0.436

0.065

0.003

pH

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Parameter

TSS (mg/L)

10

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0.161

0.014

0.001

620 nm (abs)

0.053

0.005

0.001

The flux performance was almost double when UP005 membrane was used as pre-treatment before

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NF90 membrane (Fig. 3) and the flux declined from 32.6 to 20.1 LMH. The quality of the textile wastewater permeate was considerably improved and a stable permeate flux was achieved by UF+NF coupling. Gozálvez-Zafrilla et al., (2008) subjected to NF with and without UF membrane to test biologically treated thread manufacturing factory wastewater. They concluded that UF step

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considerably reduced the membrane fouling that enhanced higher flux when compared to direct NF. Beside that, conventional methods like chemical precipitation, sand filtration, adsorption, and

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ozonation can also be used as a pre-treatment step before membrane treatment.

45

UP005 UP005+NF90

40

30 25

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Flux (L/m2 h)

35

20 15 10

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5

0

5 10 15 20 25 30 35 40 45 50 55 60

Time (min)

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0

Fig. 3. Flux behavior of direct UP005 and sequential UP005+NF90 membranes for stream A

3.2. Membrane filtration for dyeing and first washing wastewater (Stream B) Textile effluent is a mixture of wastewater from the dye bath and first washing operation. The wastewater from the reactive dyeing is characterized by high salinity, high dye stuff content, high COD (because of the additives of the dye bath like acetic acid, detergents, and completing agents), high suspended solids including cotton fibers, high temperature and pH (Tehrani-Bagha et al., 2010). It could be seen the composition of the dye bath effluent (Table 1) that color and conductivity were much higher than in the case of streams A and C. It can be concluded that reuse quality criteria cannot 11

ACCEPTED MANUSCRIPT be achieved through conventional activated sludge treatment and advanced oxidation processes. Therefore, experiments were performed using direct UF, NF and combination of UF+NF under different membrane configurations.

3.2.1 Direct ultrafiltration and nanofiltration

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Initial experiment was started with UP005 membrane. 200 mL of the effluent from the spent dyeing bath and first washing operation mixture with hydrolyzed dyes; Reactive Yellow S3R, Reactive Yellow S3B, and Setazole Deep Black with high salt concentration (330 g/L) and caustic soda (100 g/L) was placed in the dead end filtration cell. The pressure was set at 5 bar at 25±1 °C. The

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UF membrane filtration experiment was run with 57.5% water recovery. Permeate was collected in a beaker and sampled after 1 h for analytical measurements. Table 5 represents the results of UP005 membrane for dyeing bath effluent.

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COD, color, and conductivity rejections for UP005 membrane were 64.5%, 80.4% (at 436 nm), and 8.8%, respectively. However, the results did not close to reuse criteria because of high COD, color, and conductivity values. UP005 permeate was tried for fabric dyeing and it was found that the ∆E value of spectrophotometer was too high. Therefore, it was not feasible to use UP005 permeate for technological purposes. Based on UP005 experimental results, it was decided to use NF200 membrane. The same experiment with higher TMP (25 bar) was performed. The NF membrane

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filtration experiments were run with 50% water recovery. The analytical results are presented in Table 5. COD and color rejection increased to more than 95%; however, salt rejection was 13.5% due to excessive presence of salt in the feed solution. It was not possible to make an experiment with NF90 membrane directly because of too high salinity in the dye bath and therefore it could not obtain any

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experimental results for NF90 membrane.

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Table 5. Analytical results of direct UP005 and NF200 membrane filtration for stream B

Parameter

Influent

UP005 permeate

NF200 permeate

10.2

10.2

9.7

TSS (mg/L)

1,208

20.5

1.05

Turbidity (FAU)

85.4

2.3

0.4

103,300

94,200

89,300

pH

Conductivity (µS/cm)

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548

70

436 nm (abs)

10.205

2.000

0.150

525 nm (abs)

11.004

2.006

0.140

620 nm (abs)

9.450

1.579

0.085

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COD (mg/L)

Flux comparison for UP005 and NF200 membranes are presented in Fig. 4. The flux for UP005 was gradually declining from 18.5 to 10.7 LMH. The flux declined from 38.6 to 17.3 LMH for NF

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200 after 1 h. It could be seen that flux performance and permeate quality of NF200 was much better

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than UP005 membrane.

45

UP005 NF200

40

30 25 20 15 10 5 0

5 10 15 20 25 30 35 40 45 50 55 60

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0

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Flux (L/m2 h)

35

Time (min)

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Fig. 4. Flux behavior of UP005 and NF200 membranes for stream B

3.2.2. Sequential membrane filtration In order to reduce high salinity, UP005 and NF200 membranes were used as pre-treatment steps for NF90 membrane to achieve the required target in terms of conductivity rejection (Fig. 5).

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Fig. 5. Sequential membrane filtration (UP005+NF200+NF90) for stream B

The values of COD, conductivity, color and other parameters are summarized in Table 6 for

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sequential membrane filtration. This scenario enhanced high efficiency for color and COD rejection as 99.4% and 99.1%, respectively. However, conductivity and pH were still high and they were major impediments in the water recycling. As expected, produced permeate from sequential membrane

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filtration did not provide required spectrophotometric results (∆E ˃1.00). Therefore, it was not feasible to use NF90 membrane for dye bath wastewater treatment because of its high salinity.

Table 6. Analytical results of sequential membrane filtration (UP005+NF200+NF90) for stream B Influent

UP005 permeate

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Parameter

NF200 permeate

NF90 permeate

10.2

10.2

9.3

8.4

TSS (mg/L)

1,208

20.5

1.0

0.0

Turbidity (FAU)

85.4

2.3

3.4

0.0

103,300

94,200

77,500

58,700

(µS/cm)

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Conductivity

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pH

COD (mg/L)

1,546

548

138

13

436 nm (abs)

10.205

2.000

0.251

0.057

525 nm (abs)

11.004

2.006

0.192

0.032

620 nm (abs)

9.450

1.579

0.073

0.011

The flux performance is represented in Fig. 5. The flux performance was improved when UP005 membrane was used as pre-treatment step before NF200 and NF90 membrane. It should be 14

ACCEPTED MANUSCRIPT remembered that NF90 membrane could not use directly for treatment of dyeing and first washing wastewater. However, it was used after sequential membrane filtration using UP005 and NF200 membranes.

70 UP005 UP005+NF200 UP005+NF200+NF90

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60

40 30

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Flux (L/m2 h)

50

20

0

0

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10

5 10 15 20 25 30 35 40 45 50 55 60

Time (min)

Fig. 5. Flux behavior of direct UP005, sequential UP005+NF200, and sequential

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UP005+NF200+NF90 membranes for stream B

3.3. Membrane filtration for post washing wastewater (Stream C) Post washing wastewater is categorized under low concentrated waste streams. Salts and caustic

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soda are used in pre-treatment process and dyeing stages. Rinsing/washing wastewater offers a lot of potential for onsite recycling. In our study, NF90 membrane were found to be the most suitable option for rinsing/washing wastewater recovery. The results showed that NF90 permeate can be used

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anywhere in textile production cycle.

3.3.1. Direct ultrafiltration and nanofiltration Rinsing/washing wastewater (200 mL) was subjected to UP005 membrane at 5 bar TMP at 25±1 °C. The UF and NF membrane experiements were carried out 65% and 69% water recovery, respectively. The average values of the main analytical parameters for permeate samples are reported in Table 7. In this scenario, the rejection of COD and color was 80.0% and 98.4%, respectively. Conductivity rejection was low (22.0%) because of large pore size of UP005 membrane. In order to further improve of the permeate quality (Table 7), direct NF90 membrane was used at 25 bar TMP and at 25±1 °C. The permeate color was almost undetectable and turbidity, conductivity, COD, and 15

ACCEPTED MANUSCRIPT other parameters suggested a high reusability potential in textile industry process. The reusability of the permeate was confirmed by laboratory scale dyeing process and compared quality of reclaimed water dyeing with standard water dyeing using spectrophotometer. Spectrophotometric results (∆E) were found 0,99 which was under acceptable limit.

UP005 permeate

NF90 permeate

pH

8.1

7.9

6.9

TSS (mg/L)

440

2.3

Turbidity(FAU)

38.6

Conductivity (µS/cm)

3,400 559

436 nm (abs)

3.303

525 nm (abs)

3.501 2.103

0.0

0.0

2,650

214

112

9

0.054

0.004

0.056

0.004

0.035

0.002

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620 nm (abs)

2.3

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COD (mg/L)

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Influent

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Parameter

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Table 7. Analytical results of direct UP005 and NF90 membrane filtration for stream C

Flux comparison for UP005 and NF90 membranes are presented in Fig. 6. The flux for UP005 declined from 35.3 to 28.4 LMH. However, the flux declined from 37.8 to 25.1 LMH for NF90 after 1

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h. It could be seen that flux performance of UP005 membrane was better than NF90 membrane but permeate quality of NF90 was much better than UP005 membrane.

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ACCEPTED MANUSCRIPT 45 UP005 NF90

40

30

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25 20 15 10 5 0

0

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Flux (L/m2 h)

35

5 10 15 20 25 30 35 40 45 50 55 60

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Time (min)

Fig. 6. Flux behavior of UP005 and NF90 membranes for stream C

3.3.2. Sequential membrane filtration

Sequential membrane filtration was carried out using UP005 membrane as pre-treatment step

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before NF90 membrane filtration (Fig. 7). NF90 membrane performance both in terms of permeate

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quality and flux was improved when UP005 membrane was used as pre-treatment step.

Figure 7. Sequential membrane filtration (UP005+NF90) for stream C

COD, color, and conductivity rejection of the stream C using UP005+NF90 membranes are shown in Table 8. More than 99.0% of COD and color rejection were observed using NF 90 membrane at 25 bar TMP. It could be also observed that an important improvement was occurred for conductivity rejection (94.0%). These results demonstrated that NF90 membrane both individual and sequential 17

ACCEPTED MANUSCRIPT highly improved the post rinsing/washing wastewater quality. Dyeing trials at laboratory scale enhances highly promising results with ∆E value 0,603 which provided strong justification for reusing of the permate back into the process.

Table 8. Analytical results of sequential membrane filtration (UP005+NF90) for stream C UP005 permeate

NF90 permeate

pH

8.1

7.9

6.8

TSS (mg/L)

440

2.3

Turbidity (FAU)

38.6

Conductivity (µS/cm)

3,400 559

436 nm (abs)

3.303

525 nm (abs)

3.501

620 nm (abs)

2.103

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COD (mg/L)

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Influent

0.0

2.3

0.0

2,650

202

112

5

0.054

0.009

0.056

0.012

0.035

0.008

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Parameter

Flux behavior of UP005 and NF90 membranes are presented in Fig. 8. The flux for UP005

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declined from 35.3 to 28.4 LMH. Initial flux was better than direct NF90 membrane; however, it

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declined more sharply from 50.5 to 35.3 LMH after 1 h.

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60 55 50 45 40 35 30 25 20 15 10 5 0

0

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Flux (L/m2 h)

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5 10 15 20 25 30 35 40 45 50 55 60

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Time (min)

Figure 8. Flux behavior of direct UP005 and sequential UP005+NF90 membranes for stream C

3.4. Membrane treatment cost

Cost of the membrane system depends upon size of the plant, required membrane quality, membranes’ specifications, and effluent quality. Investment cost required for installation of UF and treatment systems for volumetric flow rate (Q) could be calculated capital cost (C) using

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NF

following mathematical relation according to Eq. (3) and Eq (4), respectively (ElDefrawy and Shaalan, 2007).

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C = 5159 × Q 0.62 C = 405 × Q1.0014

(3) (4)

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In accordance to this relationship, the total estimated cost for 2500 m3/day effluent discharge capacity (assuming 90% recovery for UF and 75% recovery for NF) would be 617,901 and 767,430 US$. The cost of concentrate treatment was not included. According to the literature, operational and maintenance (O & M) cost varies between 0.04-0.2 and 0.1 US$/m3 for UF and NF system, respectively (ElDefrawy and Shaalan, 2007). In our study, the project costs were estimated for post washing wastewater treatment and recovery (stream C). The capital and operating cost indicators for the NF system are shown in Table 9. The total cost for wastewater treatment was calculated 0.274 US$/m3. It was assumed that UF+NF peocesses was to be apply sequentially, construction cost for UF process was neglected in this study. As a result, total capital cost for NF process to treat and recover of wastewater from the selected batch of cotton dyeing textile industry was estimated as 1,043,375 US$.

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Table 9. Basis of capital and O & M costs estimates for the adopted treatment/recovery scheme Item/process *

Value

Cost

Reference

1. Design criteria 2.500 m3/d

-

capacity of fabric

Avarage flux

40 L/m2 h

-

experimental

Backwash

45 L/h

-

estimated

Recovery rate

70%

-

experimental

Feed pump horsepower

2.2 hp

-

calculated

Number of elements

54

-

Number of units

9

-

Feed pump electricity consumption

19.8 kWh

Capital cost of one unit

50,000 US$

Staff

3 person/day

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2. Capital costs

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Capacity

-

calculated

-

estimated

-

estimated

450,000 US$

calculated

-

Installation cost

-

500,000 US$

estimated

-

22,500 US$

5% of total capital cost of units

-

23,625 US$

5% of units and miscellaneous items

-

47,250 US$

10% of units and miscellaneous items

Miscellaneous items Plant interconnecting piping

Total capital cost **

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3. O & M costs

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Engineering

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Total capital cost of units

1,043,375 US$

Electricity

0.1 US$/kWh

47.5 US$/d

Energy Market Regulatory Authority

Labor

12.2

36.6 US$/d

Turkish Istatistical Institute

600 US$/d

estimated

Chemicals (acid, caustic, sodium hypochlorite, anti scalant) Total O & M cost ***

US$/d/person 0.5 US$/L

684 US$/d 0.274 US$/m3

* These items and costs varies considerably according to country, land site, government regulations, and labor cost ** Total capital cost did not include indirect cost such as interest rate during construction, contingency, fees, project

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4. Conclusion

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The membrane treatment system coupled with ultrafiltration as a pre-treatment was evaluated to be the most attractive option to achieve the water quality required for water reuse applications in textile wet processing industry for pre-treatment and post washing wastewater. For UF+NF sequential arrangements, color, COD, and conductivity rejection was almost 99.0% both pre-treatment and post washing wastewater and dyeing trials at lab scale provided strong encouragment for reuse potential in

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the textile wet processing. Dyeing and first washing wastewater was highly concentrated and it could be treated effectively with UP005+NF200+NF90 sequantail arrangements meet the discharge limits.

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However, the treated effluent from dyeing and first washing wastewater was not suitable for reuse into the textile wet processing because of extreme conductivity.

In the near future, water scarcity because of ground water levels decline becomes one of the main problems for many textile companies in Turkey and water consumption permits will be regulated by the government. Therefore, the textile companies that consume large volumes of water will have to improve wastewater quality to the fresh water standards for reuse purpose. The membrane process is

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one of the best alternatives to achieve sustainability water recovery from wastewater, to prevent water pollution, to reduce excessive water consumption and to protect ground water reserves for future. It is believed that the results obtained in this study will be useful for similar textile industries to recover

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References

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segregated wastewater streams.

Alcaina-Miranda, M.I., Barredo-Damas, S., Bes-Piá, A., Iborra-Clar, M.I., Iborra-Clar, A., MendozaRoca, J.A., 2009. Nanofiltration as a final step towards textile wastewater reclamation. Desalination. https://doi.org/10.1016/j.desal.2008.02.028 Alkaya, E., Demirer, G.N., 2014. Sustainable textile production: a case study from a woven fabric manufacturing mill in Turkey. J. Clean. Prod. 65, 595–603. https://doi.org/10.1016/j.jclepro.2013.07.008 American Public Health Association (APHA), 1999. Standard Methods for the Examination of Water & Wastewater 21st Edition [WWW Document]. Am. Public Heal. Assoc. Am. Water Work. A ssociation, Water Environ. Fed. Arora, S., 2014. Textile Dyes: It’s Impact on Environment and its Treatment. J. Bioremediation

21

ACCEPTED MANUSCRIPT Biodegrad. 05. https://doi.org/10.4172/2155-6199.1000e146 Asghar, A., Abdul Raman, A.A., Wan Daud, W.M.A., 2015. Advanced oxidation processes for in-situ production of hydrogen peroxide/hydroxyl radical for textile wastewater treatment: a review. J. Clean. Prod. 87, 826–838. https://doi.org/10.1016/j.jclepro.2014.09.010 ElDefrawy, N.M.H., Shaalan, H.F., 2007. Integrated membrane solutions for green textile industries. Desalination. https://doi.org/10.1016/j.desal.2006.03.542

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Francis, A., Sosamony, K.J., 2016. Treatment of Pre-treated Textile Wastewater using Moving Bed Bio-film Reactor. Procedia Technol. 24, 248–255. https://doi.org/10.1016/j.protcy.2016.05.033 Giwa, A., 2014. The Applications of Membrane Operations in the Textile Industry: A Review. Br. J. Appl. Sci. Technol. https://doi.org/10.9734/bjast/2012/1520

SC

Gozálvez-Zafrilla, J.M., Sanz-Escribano, D., Lora-García, J., León Hidalgo, M.C., 2008.

Nanofiltration of secondary effluent for wastewater reuse in the textile industry. Desalination 222, 272–279. https://doi.org/10.1016/j.desal.2007.01.173

M AN U

Güyer, G.T., Nadeem, K., Dizge, N., 2016. Recycling of pad-batch washing textile wastewater through advanced oxidation processes and its reusability assessment for Turkish textile industry. J. Clean. Prod. 139, 488–494. https://doi.org/10.1016/j.jclepro.2016.08.009 Hayat, H., Mahmood, Q., Pervez, A., Bhatti, Z.A., Baig, S.A., 2015. Comparative decolorization of dyes in textile wastewater using biological and chemical treatment. Sep. Purif. Technol. 154, 149–153. https://doi.org/10.1016/j.seppur.2015.09.025

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Holkar, C.R., Jadhav, A.J., Pinjari, D. V., Mahamuni, N.M., Pandit, A.B., 2016a. A critical review on textile wastewater treatments: Possible approaches. J. Environ. Manage. 182, 351–366. https://doi.org/10.1016/j.jenvman.2016.07.090 Holkar, C.R., Jadhav, A.J., Pinjari, D. V., Mahamuni, N.M., Pandit, A.B., 2016b. A critical review on

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textile wastewater treatments: Possible approaches. J. Environ. Manage. 182, 351–366. https://doi.org/10.1016/j.jenvman.2016.07.090 Hussain, T., Wahab, A., 2018. A critical review of the current water conservation practices in textile

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wet processing. J. Clean. Prod. 198, 806–819. https://doi.org/10.1016/j.jclepro.2018.07.051 Kant, R., 2012. Textile dyeing industry an environmental hazard. Nat. Sci. 04, 22–26. https://doi.org/10.4236/ns.2012.41004 Lin, J., Ye, W., Baltaru, M.-C., Tang, Y.P., Bernstein, N.J., Gao, P., Balta, S., Vlad, M., Volodin, A., Sotto, A., Luis, P., Zydney, A.L., Van der Bruggen, B., 2016. Tight ultrafiltration membranes for enhanced separation of dyes and Na 2 SO 4 during textile wastewater treatment. J. Memb. Sci. 514, 217–228. https://doi.org/10.1016/j.memsci.2016.04.057 Madhav, S., Ahamad, A., Singh, P., Mishra, P.K., 2018. A review of textile industry: Wet processing, environmental impacts, and effluent treatment methods. Environ. Qual. Manag. https://doi.org/10.1002/tqem.21538 Nadeem, K., Guyer, G.T., Dizge, N., 2017. Polishing of biologically treated textile wastewater through 22

ACCEPTED MANUSCRIPT AOPs and recycling for wet processing. J. Water Process Eng. 20, 29–39. https://doi.org/10.1016/j.jwpe.2017.09.011 Nawaz, M.S., Ahsan, M., 2014. Comparison of physico-chemical, advanced oxidation and biological techniques for the textile wastewater treatment. Alexandria Eng. J. 53, 717–722. https://doi.org/10.1016/j.aej.2014.06.007 Negro, C., Garcia-Ochoa, F., Tanguy, P., Ferreira, G., Thibault, J., Yamamoto, S., Gani, R., 2018.

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WITHDRAWN: Barcelona Declaration – 10th World Congress of Chemical Engineering, 1–5 October 2017. Chem. Eng. Res. Des. 129, 34. https://doi.org/10.1016/j.cherd.2017.10.022

Rahman, M.M., Hagare, D., Maheshwari, B., 2016. Use of Recycled Water for Irrigation of Open Spaces: Benefits and Risks. pp. 261–288. https://doi.org/10.1007/978-3-319-28112-4_17

SC

Sandin, G., Peters, G.M., 2018. Environmental impact of textile reuse and recycling – A review. J. Clean. Prod. 184, 353–365. https://doi.org/10.1016/j.jclepro.2018.02.266

Starling, M.C.V.M., Castro, L.A.S., Marcelino, R.B.P., Leão, M.M.D., Amorim, C.C., 2017.

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Optimized treatment conditions for textile wastewater reuse using photocatalytic processes under UV and visible light sources. Environ. Sci. Pollut. Res. 24, 6222–6232. https://doi.org/10.1007/s11356-016-6157-8

Tehrani-Bagha, A.R., Mahmoodi, N.M., Menger, F.M., 2010. Degradation of a persistent organic dye from colored textile wastewater by ozonation. Desalination 260, 34–38. https://doi.org/10.1016/j.desal.2010.05.004

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Vajnhandl, S., Valh, J.V., 2014. The status of water reuse in European textile sector. J. Environ. Manage. 141, 29–35. https://doi.org/10.1016/j.jenvman.2014.03.014 Varadarajan, G., Venkatachalam, P., 2016. Sustainable textile dyeing processes. Environ. Chem. Lett. 14, 113–122. https://doi.org/10.1007/s10311-015-0533-3

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Warsinger, D.M., Chakraborty, S., Tow, E.W., Plumlee, M.H., Bellona, C., Loutatidou, S., Karimi, L., Mikelonis, A.M., Achilli, A., Ghassemi, A., Padhye, L.P., Snyder, S.A., Curcio, S., Vecitis, C.D., Arafat, H.A., Lienhard, J.H., 2018. A review of polymeric membranes and processes for

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potable water reuse. Prog. Polym. Sci. 81, 209–237. https://doi.org/10.1016/j.progpolymsci.2018.01.004 Zhao, Y., Zhao, Y., Xu, H., Yang, Y., 2015. A Sustainable Slashing Industry Using Biodegradable Sizes from Modified Soy Protein To Replace Petro-Based Poly(Vinyl Alcohol). Environ. Sci. Technol. 49, 2391–2397. https://doi.org/10.1021/es504988w

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ACCEPTED MANUSCRIPT Highlights The recycling potentail of textile wastewater was studied using membrane technology

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The wastewater streams were segegrated into three different streams

•

Various combinations of membranes (UF and NF) were applied

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The UF-NF arrangement was evaluated the most attractive solution for water reuse

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•