The treatment of anionic surfactant wastewater using electrode ultrafiltration membrane bioreactor

doi:10.11949/0438-1157.20220862

Abstract

Abstract:

A large amount of anionic surfactant wastewater is produced in the process of cosmetics production. It has the characteristics of high organic concentration and easy to produce foam, which influence the treatment efficiency and stable operation of ordinary ultrafiltration membrane bioreactor (UMBR). In this study, a self-made electrode ultrafiltration membrane bioreactor (EMBR) was used to treat anionic surfactant wastewater. The effects of current intensity on the treatment efficiency of the pollutants and activated sludge properties were investigated, and the mechanism of membrane pollution was studied. The results showed that compared with the UMBR, under the action of electric field energy, the organic matter content in the filter cake layer of EMBR is lower, the transmembrane pressure difference (TMP) is reduced by about 50%, and the membrane fouling is less. When the current intensity was 10 mA, the removal rate of chemical oxygen demand (COD) and microbial activity were the highest, and were 97.92% and 41.6 mg/(g TSS·h), respectively. The organic content in the cake layer was the lowest and protein (PN), polysaccharide (PS) and humic acids (HA) were 5.6 mg/L, 8.02 mg/L and 0.85 mg/L, respectively. A relative low current intensity can promote the improvement of microbial activity and pollutant removal rate, and effectively control membrane pollution.

Key words: wastewater, reactor, electrode ultrafiltration membrane, membrane pollution, activated sludge, surfactant

摘要：

化妆品生产过程中产生大量的阴离子表面活性剂废水，具有有机物浓度高和易产生泡沫的特点，影响普通超滤膜生物反应器（UMBR）的处理效果和稳定运行。采用自制的电极超滤膜生物反应器（EMBR）处理阴离子表面活性剂废水，考察电流强度对EMBR污染物处理效果和活性污泥性质的影响，探索膜污染的机理。结果表明：与UMBR相比，在电场能的作用下，EMBR滤饼层的有机物含量较低，跨膜压差（TMP）降低50%左右，膜污染较轻。当电流强度为10 mA时，COD去除率和微生物活性最高，分别为97.92%和41.6 mg/（g TSS·h）；滤饼层有机物含量最低，PN、PS和HA的浓度分别为5.6、8.02、0.85 mg/L。较低的电流强度即可促进微生物活性和污染物去除率的提高，有效控制膜污染。

关键词: 废水, 反应器, 电极超滤膜, 膜污染, 活性污泥, 表面活性剂

CLC Number:

Lanhe ZHANG, Lu WANG, Zimeng LI, Hong TANG, Jingbo GUO, Yanping JIA, Mingshuang ZHANG. The treatment of anionic surfactant wastewater using electrode ultrafiltration membrane bioreactor[J]. CIESC Journal, 2022, 73(10): 4679-4691.

张兰河, 汪露, 李梓萌, 唐宏, 郭静波, 贾艳萍, 张明爽. 电极超滤膜生物反应器处理阴离子表面活性剂废水[J]. 化工学报, 2022, 73(10): 4679-4691.

Figures/Tables 12

Fig.1 Schematic diagram of experimental setup

Fig.2 TMP changes of EMBR and UMBR

Fig.3 Removal efficiencies of the pollutants in the EMBR and UMBR

Table 1 Content change of PN and PS in the EPS of activated sludge

运行阶段	反应器	PN/(mg/L)			PS/(mg/L)			EPS/(mg/L)
运行阶段	反应器	SMP	LB	TB	SMP	LB	TB	SMP	LB	TB	总量
S1	EMBR	4.61	3.82	5.60	7.07	4.76	3.49	11.68	8.58	9.09	29.35
S1	UMBR	4.61	4.22	5.40	8.33	2.55	5.70	12.94	6.76	11.10	30.80
S2	EMBR	5.60	5.20	8.17	9.07	5.60	7.70	14.67	10.80	15.87	41.34
S2	UMBR	4.02	5.01	5.99	4.97	7.70	7.91	8.99	12.71	13.91	35.61
S3	EMBR	5.20	4.81	5.40	19.38	12.43	11.38	24.58	17.24	16.78	58.60
S3	UMBR	3.82	4.61	6.19	3.28	3.18	8.86	7.10	7.79	15.05	29.94

Fig.4 3D-EEM spectra of EMBR and UMBR

Fig.5 Fourier transform infrared spectra of activated sludge

Fig.6 The properties of activated sludge in the mixed liquid and the sludge in the cake layer

Fig.7 Organic concentration in cake layer

Fig.8 Element distribution of cake layer

Table 2 The change of contact angle and Zeta potential of activated sludge

运行阶段	反应器	Zeta电位/mV	接触角/(°)
运行阶段	反应器	Zeta电位/mV	纯水	甘油	二碘甲烷
S1阶段	EMBR	-39.48	70.06	87.81	37.83
S1阶段	UMBR	-42.22	79.10	92.62	38.40
S2阶段	EMBR	-35.28	72.54	89.97	40.31
S2阶段	UMBR	-38.32	80.11	91.91	41.11
S3阶段	EMBR	-35.51	83.91	95.65	38.88
S3阶段	UMBR	-36.03	85.04	94.77	39.60
PVDF膜	未污染膜	-34.18	61.77	52.84	46.29

Fig.9 Function curve of separation distance and specific interaction energy between membrane and sludge flocs (sludge flocs size of 3 μm, pH 7.0 and temperature 293.15 K)

Fig.10 Comparison of separation distance and specific interaction energy between membrane and sludge flocs

References 34

1	Arnaldos M, Pagilla K. Effluent dissolved organic nitrogen and dissolved phosphorus removal by enhanced coagulation and microfiltration[J]. Water Research, 2010, 44(18): 5306-5315.
2	Beschkov V, Velizarov S, Agathos S N, et al. Bacterial denitrification of waste water stimulated by constant electric field[J]. Biochemical Engineering Journal, 2004, 17(2): 141-145.
3	宓益磊, 樊金红, 马鲁铭. 电-生物强化技术在水处理中的应用[J]. 水处理技术, 2009, 35(1): 34-38.
	Mi Y L, Fan J H, Ma L M. Application of bioelectrochemical technology in wastewater treatment[J]. Technology of Water Treatment, 2009, 35(1): 34-38.
4	Chang Y H D, Grodzinsky A J, Wang D I C. Augmentation of mass transfer through electrical means for hydrogel-entrapped Escherichia coli cultivation[J]. Biotechnology and Bioengineering, 1995, 48(2): 149-157.
5	She P, Song B, Xing X H, et al. Electrolytic stimulation of bacteria Enterobacter dissolvens by a direct current[J]. Biochemical Engineering Journal, 2006, 28(1): 23-29.
6	陈树德, 张红锋, 陈家森, 等. 低频电磁场对细胞生物效应的研究[J]. 中华物理医学杂志, 1998(2): 78-80.
	Chen S D, Zhang H F, Chen J S, et al. Study on biological effects of low frequency electromagnetic fields on cell[J]. Chinese Journal of Physical Medicine, 1998(2): 78-80.
7	Gregory K B, Bond D R, Lovley D R. Graphite electrodes as electron donors for anaerobic respiration[J]. Environmental Microbiology, 2004, 6(6): 596-604.
8	Pous N, Koch C, Vilà-Rovira A, et al. Monitoring and engineering reactor microbiomes of denitrifying bioelectrochemical systems[J]. RSC Advances, 2015, 5(84): 68326-68333.
9	冯小晏, 冯华军, 汪美贞, 等. 生物耦合技术在水处理中的应用[J]. 科技通报, 2012, 28(3): 139-142.
	Feng X Y, Feng H J, Wang M Z, et al. Application of bio-electrochemical technology in wastewater treatment[J]. Bulletin of Science and Technology, 2012, 28(3): 139-142.
10	Skadberg B, Geoly-Horn S L, Sangamalli V, et al. Influence of pH, current and copper on the biological dechlorination of 2, 6-dichlorophenol in an electrochemical cell[J]. Water Research, 1999, 33(9): 1997-2010.
11	李玉平, 曹宏斌, 张懿. 生物电催化方法处理三氯乙酸的研究[J]. 环境科学, 2005, 26(4): 55-58.
	Li Y P, Cao H B, Zhang Y. Reductive dechlorination of trichloroacetic acid by bioelectrochemically catalytic method[J]. Environmental Science, 2005, 26(4): 55-58.
12	竺云波, 许炉生, 吴伟勇, 等. 生物膜电极反应器降解苯胺的研究[J]. 环境污染与防治, 2009, 31(10): 61-63.
	Zhu Y B, Xu L S, Wu W Y, et al. Study on the degradation of aniline by biofilm electrode reactor[J]. Environmental Pollution ＆ Control, 2009, 31(10): 61-63.
13	康博, 黄卫民, 张应玖, 等. 生物膜电极反应器降解对氨基二甲基苯胺的研究[J]. 高等学校化学学报, 2007, 28(3): 556-558.
	Kang B, Huang W M, Zhang Y J, et al. Studies on the 4-amino-dimethyl-aniline hydrochloride degraded by a bio-electro reactor[J]. Chemical Journal of Chinese Universities, 2007, 28(3): 556-558.
14	王雪峰, 李建宏, 马宇翔, 等. 微电解水处理器的杀菌作用研究[J]. 给水排水, 2001, 27(11): 40-42.
	Wang X F, Li J H, Ma Y X,et al. Study on sterilization effect of micro-electrolyser on bacteria[J]. Water ＆ Wastewater Engineering, 2001, 27(11): 40-42.
15	钟方丽, 曹宏斌, 李鑫钢. 外电场作用下的生物膜传质模型[J]. 吉林化工学院学报, 2003, 20(4): 59-61.
	Zhong F L, Cao H B, Li X G. Study on the model of mass transfer within biofilm under electric field[J]. Journal of Jilin Institute of Chemical Technology, 2003, 20(4): 59-61.
16	Zhang L H, Zhang M S, Guo J B, et al. Effects of K⁺ salinity on the sludge activity and the microbial community structure of an A²O process[J]. Chemosphere, 2019, 235: 805-813.
17	Zhang W J, Cao B D, Wang D S, et al. Influence of wastewater sludge treatment using combined peroxyacetic acid oxidation and inorganic coagulants re-flocculation on characteristics of extracellular polymeric substances (EPS)[J]. Water Research, 2016, 88: 728-739.
18	Kühnl W, Piry A, Kaufmann V, et al. Impact of colloidal interactions on the flux in cross-flow microfiltration of milk at different pH values: a surface energy approach[J]. Journal of Membrane Science, 2010, 352(1/2): 107-115.
19	Shen L G, Lei Q, Chen J R, et al. Membrane fouling in a submerged membrane bioreactor: impacts of floc size[J]. Chemical Engineering Journal, 2015, 269: 328-334.
20	Zhang L H, Wang L, Zhang Y N, et al. The performance of electrode ultrafiltration membrane bioreactor in treating cosmetics wastewater and its anti-fouling properties[J]. Environmental Research, 2022, 206: 112629.
21	任晓克. 多维电极生物膜工艺反硝化脱氮性能研究[D]. 北京: 北京工业大学, 2015.
	Ren X K. Study on denitrification performance of multi-electrode biofilm process[D]. Beijing: Beijing University of Technology, 2015.
22	Blumer-Schuette S E, Kataeva I, Westpheling J, et al. Extremely thermophilic microorganisms for biomass conversion: status and prospects[J]. Current Opinion in Biotechnology, 2008, 19(3): 210-217.
23	Liu X W, Sheng G P, Yu H Q. Physicochemical characteristics of microbial granules[J]. Biotechnology Advances, 2009, 27(6): 1061-1070.
24	Cao B D, Zhang W J, Du Y J, et al. Compartmentalization of extracellular polymeric substances (EPS) solubilization and cake microstructure in relation to wastewater sludge dewatering behavior assisted by horizontal electric field: effect of operating conditions[J]. Water Research, 2018, 130: 363-375.
25	Wang Z P, Zhang T. Characterization of soluble microbial products (SMP) under stressful conditions[J]. Water Research, 2010, 44(18): 5499-5509.
26	柳丽芬, 赵树昌, 邓贻钊. 活性污泥化学组成的分析[J]. 环境科学, 1990, 11(2): 45-48, 96.
	Liu L F, Zhao S C, Deng Y Z. Analysis of chemical composition of activated sludge[J]. Environmental Science, 1990, 11(2): 45-48, 96.
27	D'Abzac P, Bordas F, Hullebusch E, et al. Extraction of extracellular polymeric substances (EPS) from anaerobic granular sludges: comparison of chemical and physical extraction protocols[J]. Applied Microbiology and Biotechnology, 2010, 85(5): 1589-1599.
28	Zhu L, Qi H Y, Lv M L, et al. Component analysis of extracellular polymeric substances (EPS) during aerobic sludge granulation using FTIR and 3D-EEM technologies[J]. Bioresource Technology, 2012, 124: 455-459.
29	Zhang P, Chen Y P, Guo J S, et al. Adsorption behavior of tightly bound extracellular polymeric substances on model organic surfaces under different pH and cations with surface plasmon resonance[J]. Water Research, 2014, 57: 31-39.
30	王琰, 钱飞跃, 王建芳, 等. 亚硝化颗粒污泥中EPS提取方法与组成特性的比较研究[J]. 环境科学学报, 2015, 35(11): 3515-3521.
	Wang Y, Qian F Y, Wang J F, et al. Comparative study on extraction methods and composition of extracellular polymeric substances(EPS) in granular nitrosation sludge[J]. Acta Scientiae Circumstantiae, 2015, 35(11): 3515-3521.
31	张银会, 王静, 林于廉, 等. 基于激光粒度校正的活性污泥粒径分析方法[J]. 中国给水排水, 2016, 32(17): 85-89.
	Zhang Y H, Wang J, Lin Y L, et al. Optimization method for activated sludge size analysis based on laser particle size correction[J]. China Water ＆ Wastewater, 2016, 32(17): 85-89.
32	Wang Z W, Wu Z C, Yin X, et al. Membrane fouling in a submerged membrane bioreactor (MBR) under sub-critical flux operation: membrane foulant and gel layer characterization[J]. Journal of Membrane Science, 2008, 325(1): 238-244.
33	蒋波. 阳离子型表面活性剂对活性污泥脱水性能的影响及作用机理研究[D]. 上海: 上海交通大学, 2007.
	Jiang B. Research on the effect and mechanism of cationic surfactants on the dewaterability of activated sludge[D]. Shanghai: Shanghai Jiao Tong University, 2007.
34	Liwarska-Bizukojc E, Bizukojc M. Digital image analysis to estimate the influence of sodium dodecyl sulphate on activated sludge flocs[J]. Process Biochemistry, 2005, 40(6): 2067-2072.

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