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Open AccessArticle

Brine Recycling from Industrial Textile Wastewater Treated by Ozone. By-Products Accumulation. Part 1: Multi Recycling Loop

by Lucyna Bilińska 1,*, Kazimierz Blus 1, Marta Gmurek 2 and Stanisław Ledakowicz 2
1
Textile Company Bilinski, Mickiewicza 29, 95-050 Konstantynow Lodzki, Poland
2
Faculty of Process & Environmental Engineering, Lodz University of Technology, Wolczanska 213, 90-924 Lodz, Poland
*
Author to whom correspondence should be addressed.
Water 2019, 11(3), 460; https://doi.org/10.3390/w11030460
Received: 8 January 2019 / Revised: 27 February 2019 / Accepted: 28 February 2019 / Published: 5 March 2019
(This article belongs to the Special Issue Advanced Oxidation Technologies in Industrial Wastewater Treatment)
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Abstract

The “reactive” dyeing of textiles requires an application of low-molecular-weight salts (LMWS), such as NaCl or Na2SO4, as necessary auxiliary agents. LMWS acts only as a remediation factor and remains in the dyeing effluents constitute brine. The main goal of the presented study was to investigate the application of ozone technology for industrial textile wastewater highly polluted by LMWS. The study was divided into two parts. In Part 1, by-products accumulated during multi-recycling of the same wastewater was investigated. While Part 2 was devoted to the scaling up of ozonation process, Part 1 concerns the efficiency of textile wastewater ozonation carried out as a repeatable process. The sequence of wastewater treatment and textile dyeing was repeated four times in a closed loop using the same process water. Although the wastewater decolorization was efficient in the subsequent ozonation cycles, some adverse effects, such as an increase in chemical oxygen demand (COD) and self-buffering at pH 9.5–10.0, were suggested the accumulation of by-products. The preliminary detection of by-products by thin layer chromatography (TLC) revealed phenol and naphthol derivatives as the transformation products (TPs) of ozonation. Dyeing of cotton using purified wastewater (brine) resulted in very good DECMC color matching parameters (under 1.16), but only in the first recycling loop, and then the TPs affected the process.
Keywords: ozone treatment; industrial textile wastewater; wastewater recycling; brine production from wastewater; by-products of ozonation ozone treatment; industrial textile wastewater; wastewater recycling; brine production from wastewater; by-products of ozonation

1. Introduction

About 97% of the world’s water resources are salty, which makes the water undrinkable, and less than 1% water is potable. Unfortunately, the volume of the potable water used in industry and farming is still increasing, and numerous regions on our planet suffer from a water deficit [1]. Moreover, many industrial branches produce salty wastewater that contains a huge concentration of low-molecular-weight salt (LMWS), like NaCl and Na2SO4. Therefore, a large amount of LMWS is emitted into the environment, which disturbs living conditions in the biosphere [2,3].
As far as salty wastewater is concerned, the textile industry is one of the greatest polluters. LMWSs are commonly used in dyeing processes as auxiliaries—even 1.5 kg of LMWS per 1 kg of textiles can be used in these operations [4,5,6,7]. It should be kept in mind that during industrial dyeing by reactive dyes, the application of LMWS is inherent. LMWSs are remediating agents, which increase a dye distribution from the dyebath into the textile material by changing the equilibrium conditions of the dyeing liquor [8]. Therefore, LMWS cannot be eliminated from a typical exhaustion-fixation dyeing process. Consequently, thousands of tons of LMWS are used daily by textile manufacturers [2]. The regions of huge areas, like the Panjab region in India, have been polluted by the emission of textile wastewater released into the environment, without any previous purification, which increases general salinity of surface water [3].
It is difficult to find an efficient and inexpensive treatment method that could be used to clean wastewater polluted by LMWS. Especially, biological treatment, which is the most commonly used method, could be severely affected by a high concentration of LMWS. The use of membrane filtration methods could be an option to deal with salinity; however, among them, reverse osmosis (RO) is the only method that can eliminate LMWS from wastewater. On the other hand, RO is not suitable for COD removal from wastewater because of fouling. The use of microfiltration (MF) or ultrafiltration (UF) as a pretreatment step before nanofiltration (NF) and RO is possible, but this solution cannot eliminate the fouling problem entirely. Another problem is the huge volume of highly contaminated concentrate and backwashes. At present, the operating cost of membrane filtration is still high when industrial wastewater treatment is concerned [9].
An application of ozone as a non-discharge treatment method can be an alternative for the purification of textile wastewater contaminated by LMWS. In contrast to membrane filtration, ozonation cannot remove LMWS but can serve as a technique for brine recovery from wastewater. Ozone oxidation can give good results when many poorly degradable contaminants, including textile dyes, are taken into consideration [9,10]. It can be concluded that the effectiveness of dye decomposition by ozone treatment has been proven in many papers, and the field seems to be well covered by the literature (Table 1). However, it should be noted that only a few authors have dealt with by-products detection [11,12,13,14,15], scaling-up [16], or purified wastewater recycling [17,18,19,20]. A publication that includes all these topics has not been found.
The main objective of the study presented in Part 1 was to investigate the recycling of purified wastewater. For this purpose, a highly contaminated industrial textile wastewater (the bath after the reactive dyeing of cotton, with a residual LMWS concentration equal to 30 g/L) was treated by ozone to remove color and then recycled as a source of ‘ready to use’ brine for the next dyeing. Therefore, the key idea was not to treat the LMWS as a pollutant, but as a resource that can be recycled. Consequently, the challenge was to keep LMWS concentration at a constant level, while the dye residuals were removed. To this end, the same wastewater was recycled four times (five cycles of fabric dyeing and four cycles of ozonation, carried out in a laboratory scale). The additional goal was to analyze the by-products that could have accumulated due to recycling, and their potential influence on the possibility of brine recycling.

2. Experimental

2.1. Materials

The substances used for textile dyeing and present in the wastewater were dyes and auxiliaries. The dyes were: Synozol Yellow KHL (C. I. Reactive Yellow145), Synozol Red K3BS150% (C. I. Reactive Red 195), purchased from KISCO (Eksoy Chemical Industries, Adana, Turkey), and C. I. Reactive Black 5 (purified dye, Boruta-Zachem (Bydgoszcz, Poland)). The auxiliaries were: an industrial dyeing assistant—Perigen LDR (SAA—a naphthalene sulfonic acid and carboxylates mixture, Textilchemie Dr. Petry Co. (Reutlingen, Germany)), as well as NaCl, NaOH, and Na2CO3 (technical products from Tomchem (Łódź, Poland)).
Raw knitted fabric, made of 100% cotton, was obtained from Sontex DK ApS (Ikast, Denmark); this fabric was previously bleached by a hydrogen peroxide method.

2.2. Experimental Procedure

The experiment was carried out as a sequence of textile dyeing and ozonation steps, according to the scheme presented in Figure 1.
Textile dyeing: Cotton dyeing was carried out in a LABOMAT BFA-12 system (laboratory dyeing machine made by Mathis AG, Oberhasli, Switzerland), according to a standard exhaustion-fixation procedure at a temperature of 60 °C (Figure 2). The weight of each sample was 10 g and the liquor ratio was set to 1:12. The alkalis, which were NaOH and Na2CO3 aqueous solutions, were partially dosed to avoid excessive dye hydrolyzation. The electrolyte (NaCl) was dosed only into fresh water dyes, not recycling ones.
Ozonation: A semibatch glass reactor (heterogeneous gas-liquid system) with a capacity of 1 L was used during the experiment. A gas mixture containing ozone was delivered into the reaction solution through a porous plate. Mixing was performed with a magnetic stirrer (type ES 21, Wigo, Pruszków, Poland). Ozone was produced by an Ozonek Ozone Generator (Ozonek, Lublin, Poland). The oxygen used for ozone production was supplied from a compressed gas cylinder (O2 purity 99.5%). The ozone concentration was measured at the inlet and outlet of the reactor using a BMT 963 Vent ozone analyzer. The reactor was thermostated. The temperature and pH inside of the reactor were monitored using an Elmetron C411 device (Elmetron, Zabrze, Poland). The progress of the reaction was stopped by the addition of 0.01 M Na2SO3 to the samples.

2.3. Analytical Methods

The color of the samples collected at specified time intervals was measured by a spectrophotometer (Helios Thermo Fisher Scientific, Waltham, MA, US). A calibration plot based on Lambert-Beer’s law was used to determine the concentration of the dyes in the wastewater samples.
Chemical oxygen demand (COD) was obtained using the standard method with a HACH-LANGE apparatus (DR 3800) through dichromate (VI)—LCK 514 and 314 tests.
By-product analysis was carried out by thin layer chromatography (TLC) using TLC Silica gel 60 F254 plates and ethyl acetate: n-butanol: water (1:1:8) and ethyl acetate: n-propanol: water (6:1:3) as eluents.
The colors of the textile samples were measured using a DataColor 400 reflection spectrophotometer (Datacolor AG, Dietlikon, Switzerland) in accordance with ISO 105-J03 [66]. Each measured DECMC (DE of Color Measurement Committee) value is an average of at least three measurements (measured up to a maximum error value—standard deviation from the average value set at 0.1).

3. Results and Discussion

3.1. Ozonation in a Multi Recycling Loop

After laboratory scale dyeing, the wastewater was treated by ozonation and used again in the next dyeing operation, according to the scheme presented in Figure 1. This procedure was repeated four times, which gave five cycles of dyeing (one with fresh water and four with purified brine). A brine concentration was kept at a constant level during this experiment, and after each cycle was equal to 30 g/L. Consequently, there was no need for the additional use of NaCl before subsequent dyeing in the loop.
In Figure 3, the experimental points of each ozonation processes are presented. Figure 3A shows color removal within the ozonation from cycles I to IV. It can be noted that the first ozonation (cycle I) was much more efficient in color reduction than the next ones (cycles II–IV), especially in the initial phase of the process. Therefore, the accumulation of some colorless by-products can be assumed; however, when the absorbed ozone dose is considered (Figure 3B.), the highest values were recorded for cycle IV in the final process phase. Based on this observation, it can be concluded that by-product accumulation is caused by substances inhibiting decolorization via ozonation. This accumulation not only occurs because of competitive reactions of ozone with the by-products; likely, the by-products are not as easily oxidized by the ozone as the chromophores in dye molecules. The inhibitory effect is more likely caused by the buffering of the reaction mixture (pH 9.5–10.0). A buffering effect due to the presence of ozonation by-products was observed (presented in Figure 4A). The premise for this conclusion could be the fact that NaOH concentration had to be increased in every subsequent dyeing cycle (Figure 4A) to keep the proper alkalinity. Moreover, the COD values, the initial values (before the ozone treatment), and the final values (after the ozone treatment), increased in every subsequent recycling step (Figure 4B). This observation gives information about by-product accumulation, as well.
The values of the color matching parameters of recycled textile samples, DECMC, are presented in Table 2. The standard industrial limiting value of DECMC equals 1.5 and gives information about the acceptance of color quality. It should be noted that the lowest DECMC values, under 1.16, were obtained for cycle I (the first recycling). In the cases of cycles II–IV, the DECMC values were higher, for yellow and black, above 1.5, which means that the shade was slightly changed compared to the standard (standard—textile samples dyed using fresh water). This observation could be an argument for by-product accumulation, which afterward disturbed the dyeing process. However, the DECMC values achieved by us were much more satisfying than those obtained by Hu et al. [19] during a corresponding experiment (the same number of re-dyeing cycles).
The color fastness against washing, sweat, and rubbing (in accordance with ISO 105 C06, E04, and X12, respectively [67,68,69]) of recycled textile samples was excellent, and the values were not worse than five; the reason for this result could be the respectively low depth of the tested shades, –1% (w/w).

3.2. Preliminary By-Product Study

A thin layer chromatography (TLC) was employed to a preliminary by-product analysis. The following observations could be performed while the purified wastewater was examined by TLC. Firstly, the fluorescence in the UV light, which is characteristic of naphthalene hydroxyl derivatives, was observed. Secondly, a lack of specific coloration of chromatograms after developing with Ehrlich reagent may have indicated the presence of amines. Moreover, the developing of the chromatograms with di-azo 4-nitroaniline caused the appearance of colored spots (red), which confirmed that the coupling reactions took place, and the hydroxyl aromatic compounds were present in the ozonated wastewater. At the same time, the chemical analysis carried out by a two-step process of azo-coupling (NaNO2 addition in acidic medium), and a further coupling reaction with resoricinol in a neutral medium, did not reveal the occurrence of amines. Based on TLC analysis, as well as observations of pH values during ozonation cycles (buffering phenomenon presented in Figure 4A; pKa 2-naphthol 9.51, pKa 1-naphthol 9.34, pKa phenol 9.99), it can be concluded that ozonation led to the formation of the naphthol and phenol derivatives presented in Figure 5. However, the presence of other unidentified by-products cannot be ruled out.
The formation of presented by-products is characteristic of textile wastewater ozonation in an alkaline medium. It is well known that ozone treatment under alkaline conditions leads to ozone self-decomposition, which results in the formation of hydroxyl radicals [70]. In these conditions, indirect oxidation of pollutants through hydroxyl radicals, rather than a direct one supported by ozone molecules, is the prevailing mechanism. This phenomenon drives rapid radical reactions, which are highly non-selective, and consequently, numerous low-molecular-weight by-products appear. Therefore, the presented by-products are a few of the possible ones that could have occurred. Based on the previous work of Mezzanotte et al. [71], the occurrence of various carbonyl compounds can be expected. The presence of innumerable low-molecular-weight by-products can be an explanation by low COD removal and an increase in absorbed ozone dose (discussed earlier in Section 3.1).
Our attempts to use the high performance liquid chromatography with tandem mass spectroscopy (HPLC MS/MS) analysis to confirm the occurrence of by-products did not give a satisfactory result. The presence of many low-molecular-weight by-products made the task of their identification burdensome, and any specific by-product could not be recognized in this way; however, the detection of numerous low-molecular-weight by-products favored the assumption of a radical decomposition mechanism in an alkaline reaction medium.
In accordance with the values of the DECMC parameter presented above in Table 2, it can be concluded that the identified by-products are characterized by a low affinity to cellulosic fiber materials, and the by-products’ effect on color parameters in a CIELab system is insignificant.

4. Conclusions

Based on the presented results, it can be concluded that ozonation is an efficient method for the decolorization of textile wastewater, characterized by high salinity and alkalinity. More than 90% of color removal was achieved within 30 min of the treatment. The investigation showed that the brine produced by wastewater decolorization could be successfully used in at least one subsequent dyeing of cotton fabrics. Even though the experiment indicated an efficient decolorization of textile wastewater by ozonation, the COD removal was rather poor. No more than 20% of the COD reduction could have been achieved. Correspondingly, the detected by-products, which stayed after the process, contributed low COD removal.
The multi-recycling-loop experiment indicated an accumulation of the oxidation by-products that were analyzed by TLC and chemical analysis (coupling reactions with di-azo 4-nitroaniline), as naphthol and phenol derivatives. The occurrence of these specific by-products could suggest that an indirect oxidation mechanism via free radicals can occur during ozonation of the textile wastewater. The presence of the by-products resulted in a lower color removal rate by ozone treatment in subsequent recycling loops. At the same time, the increase in the COD values and the decrease in pH values of the wastewater could be observed. The formation of a stable buffer of pH 9.5–10.0, caused by the by-product’s accumulation, could also be observed. The color shades of upcycled fabrics were slightly influenced by the occurrence of by-products. Because of the detection of by-products, the findings of this study, Part 1, encourage discussion of the industrial applicability of textile wastewater treatment by ozone. It is possible that a more complex, multi-step treatment, could result in a more efficient removal of by-products. Consequently, industrial wastewater ozonation in the upscaled system was investigated in Part 2 of the study, to determine the feasibility of industrial implementation.

Author Contributions

Conceptualization, L.B.; Methodology, L.B.; Validation, M.G. and S.L.; Investigation, L.B. and K.B.; Data curation, L.B.; Writing—original draft preparation, L.B.; Writing—review and editing, K.B., M.G. and S.L.; Supervision, M.G. and S.L.; Project administration, L.B.

Funding

This research received no external funding.

Conflicts of Interest

The authors declare no conflict of interest.

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Figure 1. Scheme of the recycling procedure (5 dyeing cycles and 4 ozonation cycles); blue—dyeing with C.I. Reactive Black 5, yellow—dyeing with C. I. Reactive Yellow145, red—dyeing with C.I. Reactive Red 195.
Figure 1. Scheme of the recycling procedure (5 dyeing cycles and 4 ozonation cycles); blue—dyeing with C.I. Reactive Black 5, yellow—dyeing with C. I. Reactive Yellow145, red—dyeing with C.I. Reactive Red 195.
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Figure 2. Reactive dyeing of cellulosic fibers according to standard exhaustion-fixation procedure run at a temperature of 60 °C.
Figure 2. Reactive dyeing of cellulosic fibers according to standard exhaustion-fixation procedure run at a temperature of 60 °C.
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Figure 3. Ozonation from cycles I to IV, Q 0.66 L/min, CO3 42.3 mg/L: (A) color removal (A/A0), (B) absorbed ozone dose mgO3/L.
Figure 3. Ozonation from cycles I to IV, Q 0.66 L/min, CO3 42.3 mg/L: (A) color removal (A/A0), (B) absorbed ozone dose mgO3/L.
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Figure 4. Ozonation cycles I–IV: (A) initial and final pH values, NaOH concentrations g/100gtextiles, (B) initial and final COD values, mgO2/L.
Figure 4. Ozonation cycles I–IV: (A) initial and final pH values, NaOH concentrations g/100gtextiles, (B) initial and final COD values, mgO2/L.
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Figure 5. Detected by-products formed during ozonation in alkaline reaction medium (based on thin layer chromatography (TLC)).
Figure 5. Detected by-products formed during ozonation in alkaline reaction medium (based on thin layer chromatography (TLC)).
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Table
Table 1. Literature overview of simulated and industrial textile wastewater treatment by ozonation. COD, chemical oxygen demand; TOC, total organic carbon; BOD, biological oxygen demand.
Table 1. Literature overview of simulated and industrial textile wastewater treatment by ozonation. COD, chemical oxygen demand; TOC, total organic carbon; BOD, biological oxygen demand.
Research GoalTextile Wastewater TypeReferences
Color, COD, TOC or BOD removalSimulated[17,21,22,23,24,25,26,27,28,29,30,31,32,33,34,35,36,37,38]
Industrial[19,39,40,41,42,43,44,45,46,47]
Kinetic studySimulated[25,26,27,30,31,33,35,37,48,49,50,51,52,53,54,55,56,57,58,59,60,61,62]
Products, degradation mechanismSimulated[11,12,13,14,15]
Salt or alkaline influenceSimulated[13,17,31,34]
Cost evaluationSimulated[27,28]
Industrial[40,43,44]
RecyclingSimulated[17]
Industrial[18,19,20]
ToxicitySimulated[23,24,27,29,61,63]
Industrial[44,45,46,64,65]
Scale upgradationIndustrial[16]
Table
Table 2. DECMC values in accordance to ISO 105-J03, when depth of shade was 1% (w/w).
Table 2. DECMC values in accordance to ISO 105-J03, when depth of shade was 1% (w/w).
Re-Dying Type of the DyeCycle No.
IIIIIIIV
Synozol Yellow KHL0.501.711.462.22
Synozol Red K3BS150%0.501.020.641.41
Setazol Black DPT1.161.921.731.56
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