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Degradation of polyvinyl alcohol in textile waste water by Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508 Jinwook Chung, Seungjin Kim, Kwangkeun Choi & Jong-Oh Kim To cite this article: Jinwook Chung, Seungjin Kim, Kwangkeun Choi & Jong-Oh Kim (2015): Degradation of polyvinyl alcohol in textile waste water by Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508, Environmental Technology, DOI: 10.1080/09593330.2015.1054257 To link to this article: http://dx.doi.org/10.1080/09593330.2015.1054257
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Date: 08 November 2015, At: 15:08
Environmental Technology, 2015 http://dx.doi.org/10.1080/09593330.2015.1054257
Degradation of polyvinyl alcohol in textile waste water by Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508 Jinwook Chunga , Seungjin Kima , Kwangkeun Choib and Jong-Oh Kimc∗ a R&D Center, Samsung Engineering Co. Ltd., 415-10 Woncheon-Dong, Youngtong-Gu, Suwon, Gyeonggi-Do 443-823, Republic of Korea; b Central Research Center, Green and Global In Tech Co. Ltd., U-Tower 910 2039, Youngduk-Dong, Kiheung-Gu, Gyeonngi-Do 446-908, Republic of Korea; c Department of Civil and Environmental Engineering, Hanyang University, 222 Wangsimni-Ro, Seongdong-Gu, Seoul, 133-791, Republic of Korea
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(Received 2 February 2015; accepted 19 May 2015 ) Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508 were isolated and identified for the degradation of polyvinyl alcohol (PVA) contained in textile waste water. Kinetic parameters such as growth rate and substrate utilization rate were determined using a pure culture of two isolated strains. The degradation rate by a mixed culture of two isolated strains was higher than that by single strain only. Also, the effect of polymerization degree on biodegradation was negligible, but initial PVA concentration was very sensitive to biodegradation. Forty-two per cent of PVA and 55% of chemical oxygen demand in textile waste water were removed by a mixed culture of two isolated strains after 5 days. Keywords: biodegradation; Microbacterium barkeri; Paenibacillus amylolyticus; polyvinyl alcohol (PVA); textile waste water
Introduction Polyvinyl alcohol (PVA) has been broadly used in various industries. Especially, it is mainly used in great amounts as a sizing agent in the textile industry. Sizing agents are used to protect the fibres from the weaving process. When the textiles are dyed, the sizing agent must be removed for increasing dyeing efficiency in the finishing process. This process results in an increase in pollutant loading, and it covers up to 60% of the entire pollutant loading from a textile finishing industry.[1,2] It was very difficult to remove PVA by simple treatment facilities, because a lot of hardly degradable materials and toxic chemicals were contained in textile waste water.[3,4] Furthermore, if membrane facility was used as a secondary treatment process, it was very important to avoid fouling problem caused by PVA. For the treatment of PVA-containing waste water, many physical and chemical treatments such as adsorption,[5] chemical coagulation,[6] ultrasonic degradation,[7,8] membrane filtration,[9] catalytic oxidation,[10,11] and Fenton’s method [12,13] have been applied, but excessive sludge was produced and the operation cost was high. Thus, many studies on the PVA degradation by using the biological method has been reported to solve these problems.[14,15] However, there is some limitations of biological treatment such as slow biodegradablility.
*Corresponding author. Email: [email protected] © 2015 Taylor & Francis
Many researchers have reported the biodegradation potential of PVA by specific microorganisms.[4,16–22] However, PVA-degrading strains isolated in most researches required the symbiotic relation and longer degrading time.[14,23,24] Few studies reported that the isolated strains were successfully applied for the waste water treatment. The purpose of this study was as follows: (1) isolation and identification of PVA-degrading strains, (2) determination of their biokinetic parameters such as growth rate and substrate utilization rate, (3) investigation of optimal conditions for PVA degradation with synthetic and industrial textile waste water and (4) comparison of removal efficiency between conventional activated sludge and a mixed culture of isolated/enriched PVA-degrading strains. Materials and methods Isolation and identification of PVA-degrading microorganisms Activated sludge sampled from the waste water treatment facilities in textile and dyeing factories consumed a lot of PVA, and it was used as a bacterial source. Medium for isolating PVA-degrading microorganism was prepared by following the composition used by Suzuki.[16] PVA was used as the sole carbon source and its polymerization
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degree was 500. Other contents were (NH4 )2 SO4 1 g, KH2 PO4 0.4 g, K2 HPO4 3.2 g, MgSO4 ·7H2 O 0.2 g, NaCl 0.1 g, FeSO4 ·7H2 O 0.01 g, yeast extract 1 g per 1 l of distilled water. pH was adjusted to 7.5 with 0.1 N NaOH and 0.1 N HCl. Shaking incubation was carried out at 28°C for 7–10 days. PVA concentration of this medium was increased step by step at each repeated culture from 0.1 to 0.3, 0.5, 0.7 and finally to 1%. Single colonies were picked from the agar plates and the PVA-degrading ability of each isolate was tested by using the agar diffusion test. The pure culture of a PVA-degrading microorganism was obtained by repeated plate cultures. The isolated strains were identified by Micro Station System (Biolog. Inc., USA). Morphological identification of the isolated strains was carried out according to Bergey’s Manual. Determination of kinetic parameter Isolated strains were pre-incubated using the abovementioned medium at 30°C and 150 rpm, and 10 mL of culture was sampled, and then the cell was obtained by centrifugation. In this case, phosphoric buffer solution (pH 7) was used for re-suspending the cell, and the inoculums were applied to the PVA biodegradation test. Culture flasks were used for the tests on a shaking incubator at 30°C under aerobic conditions. A UV/VIS spectrophotometer (Shimadzu, Japan) was used for measuring microbial growth at 660 nm. To describe the biodegradation of PVA quantitatively, it is necessary to evaluate the relationship between the specific growth rate and the concentration of substrate. It was assumed that the specific growth rate depends only on the concentration of PVA for constant pH and temperature. Generally, microbial growth and consumption rate of substrate can be expressed as a first-order equation. If it was assumed that only a substrate gives the effect to microbial growth and if other conditions were kept constant, it could be well explained by the Monod equation. The Monod equation describes a substrate-limited growth only when growth was slow and population density was low, which was expressed as μ = (μm S)/(K s + S), where μ was specific growth rate, μm was maximum specific growth rate, S was represented as concentrations of PVA and K s was half saturation concentration. Five different initial concentrations (10, 25, 50, 75 and 100 mg L−1 ) of PVA were tested for searching the biodegradability conditions of PVA. Characteristics of textile waste water Textile waste water was sampled from the S industrial complex located in Daegu, Korea. PVA and starch as sizing agents were generally used in this industrial complex. One of them, starch, was easily degraded biologically, while PVA was hardly degraded because of their characteristics such as high viscosity and strong adhesiveness to fibre. The characteristics of textile waste water were as follows:
PVA concentrations 950 mg L−1 , chemical oxygen demand (COD) 2250 mg L−1 , suspended solids 1400 mg L−1 and pH 5.1, respectively. Three types of PVA were used in textile manufacturing facilities; PVA 1799 (1700 polymerization degree), PVA588 (500 polymerization degree) and PVA124 (400 polymerization degree). Also, the real textile waste water contained low levels of toxicants such as sulphide and ammonium salts, and refractory organics such as surfactants and chlorinated organic compounds. Batch experiment Synthetic textile waste water was used to culture isolated strains. Experimental conditions for PVA degradation were pH 7 ± 0.2, 30 ± 1°C, and 150 rpm at a 500 mL acryl reactor during 5 days under aerobic conditions, and a mixed culture as the inoculate was used as 10% (v/v) of textile waste water. To evaluate the effect of polymerization degree and initial PVA concentration on PVA degradation, the synthetic waste water was prepared using different polymerization degrees (500, 1500 and 2000, respectively). Analytical method PVA in waste water was quantitatively analysed by Finley’s method.[25] When PVA concentration was measured, some factors (especially, starch) must be removed from waste water because starch gives an error which resembles a similar absorbance range to PVA. So, pre-treatment was performed to remove starch by acid hydrolysis with 0.2–0.5 N HCl solutions for 90 min under 100°C. The COD was measured by a HACH spectrophotometer DR/2010 using the COD reactor digestion method. The mixed liquor suspended solid (MLSS), TN, TP and oxygen uptake rate (OUR) were measured by standard methods for the examination of water and waste water.[26] Result and discussion Isolation and identification microorganisms Thirty-four different strains were isolated from textile waste water and sludge. Results of the PVA degradation test using these strains are shown in Figure 1. As shown in Figure 1, the PVA-degrading efficiency was obtained ranging from 22% to 98%. According to the results, two strains among them (represented 28 and 34 in Figure 1) were finally isolated and after identification, they were named as Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508, respectively. These two isolated strains were used for further study. Determination of kinetic parameter Biodegradation efficiencies of two isolated strains were very similar to each other, but specific biodegradation rate
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Figure 1. Biodegradation of PVA by 34 different strains (28: P. amylolyticus KCCM 10508, 34: M. barkeri KCCM 10507).
of P. amylolyticus KCCM 10508 was a little higher (1.2 times) than that of M. barkeri KCCM 10507. Specific growth rates (μ) of them were measured to find the kinetic data for PVA biodegradation. Because μ is a function of substrate concentration, it was measured during exponential growth phase and the concentration of PVA did not change significantly with time during that phase. To calculate specific growth rate more precisely, six different initial concentrations of PVA were used. As shown in Figure 2, experimental data were fitted to the Monod model by using the least-squares method. From this result, the maximum specific growth rates (μm ) were obtained as 0.213 and 0.207 h−1 for M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508, respectively. The Monod equation can be applied to describe the dependence of specific growth (or biodegradation) rate with the concentration of PVA. Biokinetic constant in this model wase estimated by numerical approaches. Figure 3 shows simulation results of experimental data by using M. barkeri KCCM 10507 and P. amylolyticus
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KCCM 10508, respectively. Numerical simulation showed good fits to the experimental data with predicted values, μm = 0.213 h−1 , K s = 5.4 mg L−1 and Yx/s = 0.046 OD biomass/mg PVA by M. barkeri KCCM 10507, and μm = 0.207 h−1 , K s = 5.6 mg L−1 and Yx/s = 0.037 OD biomass/mg PVA for P. amylolyticus KCCM 10508, respectively. Many researches on biodegradation of PVA by using isolated strains were previously reported, and the biodegradability results of some works are summarized in Table 1. Specific biodegradation rate was calculated from the amount of PVA degraded and the time required for PVA biodegradation. As shown in Table 1, the specific biodegradation rate obtained in this study was higher than others. That is, the specific biodegradation rate of 4.1– 4.2 mg L−1 h−1 was obtained in this study, while it was ranging from 0.4 to 3.8 mg L−1 h−1 in other works. These results indicated that two strains isolated in this study have good ability for PVA degradation. So, it was concluded that these two strains could be used to efficiently treat PVA-containing waste water like textile waste water. As mentioned above, the kinetic constants (μm and K s ) of two isolated strains were higher than other reports, although it was more difficult to degrade PVA than oligomer of PVA or 4,6-nonanediol due to its complicated structure and saponification. These results also indicated that M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 could be useful strains for the biodegradation of PVA.
Comparison of PVA degradation efficiency Textile waste water containing PVA was tested to compare the results of PVA degradation efficiency by using a mixed culture of two isolated strains (mixture ratio 1:1 based on dry weight) or single strain only. As shown in Figure 4, a mixed culture has a good ability for degrading PVA, and PVA degradation efficiency was also high even if a single strain was used. As a result, PVA-degrading percentage by
Figure 2. Specific growth rate (μ) as a function of the initial concentration of PVA (S 0 ) by (a) M. barkeri KCCM 10507 and (b) P. amylolyticus KCCM 10508.
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Figure 3. Comparison between model prediction and experimental data for biomass and concentration of PVA at 50 mg L−1 by (a) M. barkeri KCCM 10507 and (b) P. amylolyticus KCCM 10508. Table 1. Specific biodegradation rate of PVA by using isolated strains under aerobic condition. Concentration of PVA (mg L−1 ) Strains Bacillus megaterium Pseudomonas O-3 Pseudomonas sp. Pseudomonas cepacia Pseudomonas sp. A-41 Pasteurella haemolytica Cardiobacterium sp. SB68 M. barkeri KCCM 10507 P. amylolyticus KCCM 10508
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[14] [16] [17] [20] [4] [19] [21] This study This study
M. barkeri KCCM 10507, P. amylolyticus KCCM 10508, and a mixed culture of two strains were obtained as 98, 96 and 99%, respectively. So, it was concluded that these two strains have an excellent ability for degrading PVA whether a single strain only or a mixed culture was used.
Effect of polymerization degree and initial PVA concentration on PVA degradation The effect of polymerization degree of PVA on biodegradation was tested by using a mixed culture of two strains. In this experiment, the initial PVA concentration was fixed at 1000 mg L−1 . It was generally reported that PVA degradation rate was decreased with increasing polymerization degree. So, three different types of PVA which have 500, 1500 and 2000 of the polymerization degree were used in this test. As shown in Figure 5(a), PVA-degrading rates in the cases of 500 and 1500 polymerization degrees rose quickly and went to over 90% degradation after 4 days. On the other hand, the degradation rate in the case of 2000 polymerization degree rose slower than the other cases and increased to about 80% degradation in 5 days. Although less PVA degradation was observed in the case of
Figure 4. Biodegradation of PVA contained in the synthetic waste water by the single culture and mixed culture of M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508.
2000 polymerization degree, polymerization degree does not seem to have a great effect on the degradation ability of M. barkeri KCCM 10507 and P. amylolyticus KCCM
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10508 up to 2000 polymerization degrees to apply to the waste water treatment processes. These results are similar to the data reported by Suzuki et al. [16] that there was no effect of polymerization degree on the PVA degradation by using Pseudomonas sp. As a result, it was considered that polymerization degree have little effect on PVA degradation rate and microbial growth. Various initial concentrations of PVA were tested to find the effect of initial concentration of PVA on biodegradation by using M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508. The initial concentration varies between 50 and 3500 mg L−1 and polymerization degree of PVA used for this test was 500 because it was used most extensively in the textile industries. If initial concentration of PVA was below than 750 mg L−1 , about 90% of PVA could be degraded. When 1500 mg L−1 PVA above was used, M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 showed much lower degradation efficiency, but this high concentration of PVA was seldom observed in the textile industries (see Figure 5(b)). Extensive published studies have established a two-step process for the biodegradation of PVA. The first step is either (1) oxidation of two adjacent hydroxyl groups leading to β-diketone structures or (2) oxidation
of one hydroxyl group yielding monoketone structures. According to the products produced by the first step, there were two possible pathways for the second step; either hydrolysis of β-diketone structures of oxidized PVA by a β-diketone hydrolase or/and the aldolase reaction involving the monoketone structures of oxidized PVA.[27–29] Based on the degradation pathway, as initial PVA concentration increases, the hydroxyl group is accumulated in the periplasmic space inside bacteria and can inhibit the activity of PVA oxidase. Effect of microbial competition on PVA degradation Figure 6 shows the results of PVA degradation in the two cases: (a) sterilized waste water and (b) non-sterilized waste water. This classification was made in order to observe whether there is some interactions between inoculated strains and original species present in the textile waste water or not. That is, this test was carried out to find whether strains isolated in this test could be used in real waste water or not. For the sterilized waste water case as shown in Figure 6(a), 50% of PVA was degraded and 72.8% of COD was removed within 5 days. During this
10 PVA COD MLSS pH
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Figure 5. Effect of (a) polymerization degree and (b) different initial concentration on PVA degradation efficiency by M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508. -1 Concentrations of PVA, COD and MLSS (mg L )
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Figure 6. Treatment efficiency of PVA and COD contained in (a) sterilized waste water and (b) textile waste water by the mixed culture of M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508.
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test, MLSS was increased from 1100 to 2200 mg L−1 , and pH was changed from 5.1 to 7.8. As a result of Figure 6(a), it was considered that M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 seemed to have a good ability of PVA degradation and COD removal. On the contrary, results in Figure 6(b) show less degradation rates compared to the results in Figure 6(a). Namely, just 30% of PVA was degraded, and 55% of COD was removed after 5 days. Changes of pH and MLSS, however, showed similar results to the case using sterilized waste water. It was considered that activity of strains inoculated was maintained even if other species was present. So, it was considered that applicability of two strains was very high, but there are some inhibition effects by other species when applied to the industrial waste water directly. PVA-degrading efficiency in this test was also different from the results when using synthetic waste water. When the initial concentration of PVA was 1000 mg L−1 in synthetic waste water, PVA degradation rate was about 90% (see Figure 5(b)). Thirty per cent of PVA, however, was degraded by using industrial waste water. That is, about 60% of PVA-degrading efficiency was different although a similar range of initial concentrations of PVA was used. This result implies that the lower efficiency in real textile waste water is caused by various inhibitory compounds such as toxicants and refractory organic compounds.[30,31] Also, at the early stage of operation, the degradation of PVA was retarded but the degradation of COD increased sharply regardless of sterilization. It was considered that easily biodegradable compounds present in the waste water were degraded preferentially rather than PVA due to the affinity of substrate. Therefore, suitable pre-treatment for sufficient adaptation of M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 seemed to be needed for increasing the PVA degradation rate. When these two strains were used, the degrading rate was 90% within 750 mg PVA L−1 , while it was gradually decreased up to 20% with increasing concentrations of PVA. When these strains were inoculated directly to textile waste water, MLSS was changed from 1400 to 2500 mg L−1 , and COD and PVA was removed to 55% and 30%, respectively.
Conclusions M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 were isolated and identified from textile waste water for efficient PVA degradation. PVA which was contained in synthetic waste water was degraded by 96% and 98% by M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508, respectively. These two strains degraded PVA regardless of the polymerization degree and showed 90% over degradation ratio when the initial concentration of PVA was below 750 mg L−1 . As the initial concentrations were increased, however, the degradation efficiency was gradually decreased to 30%. The PVA and COD in
raw textile waste water were degraded 42% and removed 55%, respectively, by a mixed culture of two strains. These results indicated that these two strains have good PVA-degrading activity as well as efficient COD removal activity. Disclosure statement No potential conflict of interest was reported by the authors.
Funding This study was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government [NRF2013R1A2A1A09007252].
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ISSN: 0959-3330 (Print) 1479-487X (Online) Journal homepage: http://www.tandfonline.com/loi/tent20
Degradation of polyvinyl alcohol in textile waste water by Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508 Jinwook Chung, Seungjin Kim, Kwangkeun Choi & Jong-Oh Kim To cite this article: Jinwook Chung, Seungjin Kim, Kwangkeun Choi & Jong-Oh Kim (2015): Degradation of polyvinyl alcohol in textile waste water by Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508, Environmental Technology, DOI: 10.1080/09593330.2015.1054257 To link to this article: http://dx.doi.org/10.1080/09593330.2015.1054257
Accepted author version posted online: 22 May 2015. Published online: 17 Jun 2015. Submit your article to this journal
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Date: 08 November 2015, At: 15:08
Environmental Technology, 2015 http://dx.doi.org/10.1080/09593330.2015.1054257
Degradation of polyvinyl alcohol in textile waste water by Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508 Jinwook Chunga , Seungjin Kima , Kwangkeun Choib and Jong-Oh Kimc∗ a R&D Center, Samsung Engineering Co. Ltd., 415-10 Woncheon-Dong, Youngtong-Gu, Suwon, Gyeonggi-Do 443-823, Republic of Korea; b Central Research Center, Green and Global In Tech Co. Ltd., U-Tower 910 2039, Youngduk-Dong, Kiheung-Gu, Gyeonngi-Do 446-908, Republic of Korea; c Department of Civil and Environmental Engineering, Hanyang University, 222 Wangsimni-Ro, Seongdong-Gu, Seoul, 133-791, Republic of Korea
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(Received 2 February 2015; accepted 19 May 2015 ) Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508 were isolated and identified for the degradation of polyvinyl alcohol (PVA) contained in textile waste water. Kinetic parameters such as growth rate and substrate utilization rate were determined using a pure culture of two isolated strains. The degradation rate by a mixed culture of two isolated strains was higher than that by single strain only. Also, the effect of polymerization degree on biodegradation was negligible, but initial PVA concentration was very sensitive to biodegradation. Forty-two per cent of PVA and 55% of chemical oxygen demand in textile waste water were removed by a mixed culture of two isolated strains after 5 days. Keywords: biodegradation; Microbacterium barkeri; Paenibacillus amylolyticus; polyvinyl alcohol (PVA); textile waste water
Introduction Polyvinyl alcohol (PVA) has been broadly used in various industries. Especially, it is mainly used in great amounts as a sizing agent in the textile industry. Sizing agents are used to protect the fibres from the weaving process. When the textiles are dyed, the sizing agent must be removed for increasing dyeing efficiency in the finishing process. This process results in an increase in pollutant loading, and it covers up to 60% of the entire pollutant loading from a textile finishing industry.[1,2] It was very difficult to remove PVA by simple treatment facilities, because a lot of hardly degradable materials and toxic chemicals were contained in textile waste water.[3,4] Furthermore, if membrane facility was used as a secondary treatment process, it was very important to avoid fouling problem caused by PVA. For the treatment of PVA-containing waste water, many physical and chemical treatments such as adsorption,[5] chemical coagulation,[6] ultrasonic degradation,[7,8] membrane filtration,[9] catalytic oxidation,[10,11] and Fenton’s method [12,13] have been applied, but excessive sludge was produced and the operation cost was high. Thus, many studies on the PVA degradation by using the biological method has been reported to solve these problems.[14,15] However, there is some limitations of biological treatment such as slow biodegradablility.
*Corresponding author. Email: [email protected] © 2015 Taylor & Francis
Many researchers have reported the biodegradation potential of PVA by specific microorganisms.[4,16–22] However, PVA-degrading strains isolated in most researches required the symbiotic relation and longer degrading time.[14,23,24] Few studies reported that the isolated strains were successfully applied for the waste water treatment. The purpose of this study was as follows: (1) isolation and identification of PVA-degrading strains, (2) determination of their biokinetic parameters such as growth rate and substrate utilization rate, (3) investigation of optimal conditions for PVA degradation with synthetic and industrial textile waste water and (4) comparison of removal efficiency between conventional activated sludge and a mixed culture of isolated/enriched PVA-degrading strains. Materials and methods Isolation and identification of PVA-degrading microorganisms Activated sludge sampled from the waste water treatment facilities in textile and dyeing factories consumed a lot of PVA, and it was used as a bacterial source. Medium for isolating PVA-degrading microorganism was prepared by following the composition used by Suzuki.[16] PVA was used as the sole carbon source and its polymerization
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degree was 500. Other contents were (NH4 )2 SO4 1 g, KH2 PO4 0.4 g, K2 HPO4 3.2 g, MgSO4 ·7H2 O 0.2 g, NaCl 0.1 g, FeSO4 ·7H2 O 0.01 g, yeast extract 1 g per 1 l of distilled water. pH was adjusted to 7.5 with 0.1 N NaOH and 0.1 N HCl. Shaking incubation was carried out at 28°C for 7–10 days. PVA concentration of this medium was increased step by step at each repeated culture from 0.1 to 0.3, 0.5, 0.7 and finally to 1%. Single colonies were picked from the agar plates and the PVA-degrading ability of each isolate was tested by using the agar diffusion test. The pure culture of a PVA-degrading microorganism was obtained by repeated plate cultures. The isolated strains were identified by Micro Station System (Biolog. Inc., USA). Morphological identification of the isolated strains was carried out according to Bergey’s Manual. Determination of kinetic parameter Isolated strains were pre-incubated using the abovementioned medium at 30°C and 150 rpm, and 10 mL of culture was sampled, and then the cell was obtained by centrifugation. In this case, phosphoric buffer solution (pH 7) was used for re-suspending the cell, and the inoculums were applied to the PVA biodegradation test. Culture flasks were used for the tests on a shaking incubator at 30°C under aerobic conditions. A UV/VIS spectrophotometer (Shimadzu, Japan) was used for measuring microbial growth at 660 nm. To describe the biodegradation of PVA quantitatively, it is necessary to evaluate the relationship between the specific growth rate and the concentration of substrate. It was assumed that the specific growth rate depends only on the concentration of PVA for constant pH and temperature. Generally, microbial growth and consumption rate of substrate can be expressed as a first-order equation. If it was assumed that only a substrate gives the effect to microbial growth and if other conditions were kept constant, it could be well explained by the Monod equation. The Monod equation describes a substrate-limited growth only when growth was slow and population density was low, which was expressed as μ = (μm S)/(K s + S), where μ was specific growth rate, μm was maximum specific growth rate, S was represented as concentrations of PVA and K s was half saturation concentration. Five different initial concentrations (10, 25, 50, 75 and 100 mg L−1 ) of PVA were tested for searching the biodegradability conditions of PVA. Characteristics of textile waste water Textile waste water was sampled from the S industrial complex located in Daegu, Korea. PVA and starch as sizing agents were generally used in this industrial complex. One of them, starch, was easily degraded biologically, while PVA was hardly degraded because of their characteristics such as high viscosity and strong adhesiveness to fibre. The characteristics of textile waste water were as follows:
PVA concentrations 950 mg L−1 , chemical oxygen demand (COD) 2250 mg L−1 , suspended solids 1400 mg L−1 and pH 5.1, respectively. Three types of PVA were used in textile manufacturing facilities; PVA 1799 (1700 polymerization degree), PVA588 (500 polymerization degree) and PVA124 (400 polymerization degree). Also, the real textile waste water contained low levels of toxicants such as sulphide and ammonium salts, and refractory organics such as surfactants and chlorinated organic compounds. Batch experiment Synthetic textile waste water was used to culture isolated strains. Experimental conditions for PVA degradation were pH 7 ± 0.2, 30 ± 1°C, and 150 rpm at a 500 mL acryl reactor during 5 days under aerobic conditions, and a mixed culture as the inoculate was used as 10% (v/v) of textile waste water. To evaluate the effect of polymerization degree and initial PVA concentration on PVA degradation, the synthetic waste water was prepared using different polymerization degrees (500, 1500 and 2000, respectively). Analytical method PVA in waste water was quantitatively analysed by Finley’s method.[25] When PVA concentration was measured, some factors (especially, starch) must be removed from waste water because starch gives an error which resembles a similar absorbance range to PVA. So, pre-treatment was performed to remove starch by acid hydrolysis with 0.2–0.5 N HCl solutions for 90 min under 100°C. The COD was measured by a HACH spectrophotometer DR/2010 using the COD reactor digestion method. The mixed liquor suspended solid (MLSS), TN, TP and oxygen uptake rate (OUR) were measured by standard methods for the examination of water and waste water.[26] Result and discussion Isolation and identification microorganisms Thirty-four different strains were isolated from textile waste water and sludge. Results of the PVA degradation test using these strains are shown in Figure 1. As shown in Figure 1, the PVA-degrading efficiency was obtained ranging from 22% to 98%. According to the results, two strains among them (represented 28 and 34 in Figure 1) were finally isolated and after identification, they were named as Microbacterium barkeri KCCM 10507 and Paenibacillus amylolyticus KCCM 10508, respectively. These two isolated strains were used for further study. Determination of kinetic parameter Biodegradation efficiencies of two isolated strains were very similar to each other, but specific biodegradation rate
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Figure 1. Biodegradation of PVA by 34 different strains (28: P. amylolyticus KCCM 10508, 34: M. barkeri KCCM 10507).
of P. amylolyticus KCCM 10508 was a little higher (1.2 times) than that of M. barkeri KCCM 10507. Specific growth rates (μ) of them were measured to find the kinetic data for PVA biodegradation. Because μ is a function of substrate concentration, it was measured during exponential growth phase and the concentration of PVA did not change significantly with time during that phase. To calculate specific growth rate more precisely, six different initial concentrations of PVA were used. As shown in Figure 2, experimental data were fitted to the Monod model by using the least-squares method. From this result, the maximum specific growth rates (μm ) were obtained as 0.213 and 0.207 h−1 for M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508, respectively. The Monod equation can be applied to describe the dependence of specific growth (or biodegradation) rate with the concentration of PVA. Biokinetic constant in this model wase estimated by numerical approaches. Figure 3 shows simulation results of experimental data by using M. barkeri KCCM 10507 and P. amylolyticus
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KCCM 10508, respectively. Numerical simulation showed good fits to the experimental data with predicted values, μm = 0.213 h−1 , K s = 5.4 mg L−1 and Yx/s = 0.046 OD biomass/mg PVA by M. barkeri KCCM 10507, and μm = 0.207 h−1 , K s = 5.6 mg L−1 and Yx/s = 0.037 OD biomass/mg PVA for P. amylolyticus KCCM 10508, respectively. Many researches on biodegradation of PVA by using isolated strains were previously reported, and the biodegradability results of some works are summarized in Table 1. Specific biodegradation rate was calculated from the amount of PVA degraded and the time required for PVA biodegradation. As shown in Table 1, the specific biodegradation rate obtained in this study was higher than others. That is, the specific biodegradation rate of 4.1– 4.2 mg L−1 h−1 was obtained in this study, while it was ranging from 0.4 to 3.8 mg L−1 h−1 in other works. These results indicated that two strains isolated in this study have good ability for PVA degradation. So, it was concluded that these two strains could be used to efficiently treat PVA-containing waste water like textile waste water. As mentioned above, the kinetic constants (μm and K s ) of two isolated strains were higher than other reports, although it was more difficult to degrade PVA than oligomer of PVA or 4,6-nonanediol due to its complicated structure and saponification. These results also indicated that M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 could be useful strains for the biodegradation of PVA.
Comparison of PVA degradation efficiency Textile waste water containing PVA was tested to compare the results of PVA degradation efficiency by using a mixed culture of two isolated strains (mixture ratio 1:1 based on dry weight) or single strain only. As shown in Figure 4, a mixed culture has a good ability for degrading PVA, and PVA degradation efficiency was also high even if a single strain was used. As a result, PVA-degrading percentage by
Figure 2. Specific growth rate (μ) as a function of the initial concentration of PVA (S 0 ) by (a) M. barkeri KCCM 10507 and (b) P. amylolyticus KCCM 10508.
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Figure 3. Comparison between model prediction and experimental data for biomass and concentration of PVA at 50 mg L−1 by (a) M. barkeri KCCM 10507 and (b) P. amylolyticus KCCM 10508. Table 1. Specific biodegradation rate of PVA by using isolated strains under aerobic condition. Concentration of PVA (mg L−1 ) Strains Bacillus megaterium Pseudomonas O-3 Pseudomonas sp. Pseudomonas cepacia Pseudomonas sp. A-41 Pasteurella haemolytica Cardiobacterium sp. SB68 M. barkeri KCCM 10507 P. amylolyticus KCCM 10508
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M. barkeri KCCM 10507, P. amylolyticus KCCM 10508, and a mixed culture of two strains were obtained as 98, 96 and 99%, respectively. So, it was concluded that these two strains have an excellent ability for degrading PVA whether a single strain only or a mixed culture was used.
Effect of polymerization degree and initial PVA concentration on PVA degradation The effect of polymerization degree of PVA on biodegradation was tested by using a mixed culture of two strains. In this experiment, the initial PVA concentration was fixed at 1000 mg L−1 . It was generally reported that PVA degradation rate was decreased with increasing polymerization degree. So, three different types of PVA which have 500, 1500 and 2000 of the polymerization degree were used in this test. As shown in Figure 5(a), PVA-degrading rates in the cases of 500 and 1500 polymerization degrees rose quickly and went to over 90% degradation after 4 days. On the other hand, the degradation rate in the case of 2000 polymerization degree rose slower than the other cases and increased to about 80% degradation in 5 days. Although less PVA degradation was observed in the case of
Figure 4. Biodegradation of PVA contained in the synthetic waste water by the single culture and mixed culture of M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508.
2000 polymerization degree, polymerization degree does not seem to have a great effect on the degradation ability of M. barkeri KCCM 10507 and P. amylolyticus KCCM
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10508 up to 2000 polymerization degrees to apply to the waste water treatment processes. These results are similar to the data reported by Suzuki et al. [16] that there was no effect of polymerization degree on the PVA degradation by using Pseudomonas sp. As a result, it was considered that polymerization degree have little effect on PVA degradation rate and microbial growth. Various initial concentrations of PVA were tested to find the effect of initial concentration of PVA on biodegradation by using M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508. The initial concentration varies between 50 and 3500 mg L−1 and polymerization degree of PVA used for this test was 500 because it was used most extensively in the textile industries. If initial concentration of PVA was below than 750 mg L−1 , about 90% of PVA could be degraded. When 1500 mg L−1 PVA above was used, M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 showed much lower degradation efficiency, but this high concentration of PVA was seldom observed in the textile industries (see Figure 5(b)). Extensive published studies have established a two-step process for the biodegradation of PVA. The first step is either (1) oxidation of two adjacent hydroxyl groups leading to β-diketone structures or (2) oxidation
of one hydroxyl group yielding monoketone structures. According to the products produced by the first step, there were two possible pathways for the second step; either hydrolysis of β-diketone structures of oxidized PVA by a β-diketone hydrolase or/and the aldolase reaction involving the monoketone structures of oxidized PVA.[27–29] Based on the degradation pathway, as initial PVA concentration increases, the hydroxyl group is accumulated in the periplasmic space inside bacteria and can inhibit the activity of PVA oxidase. Effect of microbial competition on PVA degradation Figure 6 shows the results of PVA degradation in the two cases: (a) sterilized waste water and (b) non-sterilized waste water. This classification was made in order to observe whether there is some interactions between inoculated strains and original species present in the textile waste water or not. That is, this test was carried out to find whether strains isolated in this test could be used in real waste water or not. For the sterilized waste water case as shown in Figure 6(a), 50% of PVA was degraded and 72.8% of COD was removed within 5 days. During this
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Figure 5. Effect of (a) polymerization degree and (b) different initial concentration on PVA degradation efficiency by M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508. -1 Concentrations of PVA, COD and MLSS (mg L )
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Figure 6. Treatment efficiency of PVA and COD contained in (a) sterilized waste water and (b) textile waste water by the mixed culture of M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508.
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test, MLSS was increased from 1100 to 2200 mg L−1 , and pH was changed from 5.1 to 7.8. As a result of Figure 6(a), it was considered that M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 seemed to have a good ability of PVA degradation and COD removal. On the contrary, results in Figure 6(b) show less degradation rates compared to the results in Figure 6(a). Namely, just 30% of PVA was degraded, and 55% of COD was removed after 5 days. Changes of pH and MLSS, however, showed similar results to the case using sterilized waste water. It was considered that activity of strains inoculated was maintained even if other species was present. So, it was considered that applicability of two strains was very high, but there are some inhibition effects by other species when applied to the industrial waste water directly. PVA-degrading efficiency in this test was also different from the results when using synthetic waste water. When the initial concentration of PVA was 1000 mg L−1 in synthetic waste water, PVA degradation rate was about 90% (see Figure 5(b)). Thirty per cent of PVA, however, was degraded by using industrial waste water. That is, about 60% of PVA-degrading efficiency was different although a similar range of initial concentrations of PVA was used. This result implies that the lower efficiency in real textile waste water is caused by various inhibitory compounds such as toxicants and refractory organic compounds.[30,31] Also, at the early stage of operation, the degradation of PVA was retarded but the degradation of COD increased sharply regardless of sterilization. It was considered that easily biodegradable compounds present in the waste water were degraded preferentially rather than PVA due to the affinity of substrate. Therefore, suitable pre-treatment for sufficient adaptation of M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 seemed to be needed for increasing the PVA degradation rate. When these two strains were used, the degrading rate was 90% within 750 mg PVA L−1 , while it was gradually decreased up to 20% with increasing concentrations of PVA. When these strains were inoculated directly to textile waste water, MLSS was changed from 1400 to 2500 mg L−1 , and COD and PVA was removed to 55% and 30%, respectively.
Conclusions M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508 were isolated and identified from textile waste water for efficient PVA degradation. PVA which was contained in synthetic waste water was degraded by 96% and 98% by M. barkeri KCCM 10507 and P. amylolyticus KCCM 10508, respectively. These two strains degraded PVA regardless of the polymerization degree and showed 90% over degradation ratio when the initial concentration of PVA was below 750 mg L−1 . As the initial concentrations were increased, however, the degradation efficiency was gradually decreased to 30%. The PVA and COD in
raw textile waste water were degraded 42% and removed 55%, respectively, by a mixed culture of two strains. These results indicated that these two strains have good PVA-degrading activity as well as efficient COD removal activity. Disclosure statement No potential conflict of interest was reported by the authors.
Funding This study was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government [NRF2013R1A2A1A09007252].
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