Fabrication of Bi-SnO2 electro-catalytic membrane for enhanced removal of carbamazepine in drinking water
WEI Yong1,2, GUO Zi-yin1, YUAN Xue-feng3, LI Ke-ying2, ZHOU Chen2, SUN Tian2
1. School of Environmental Science and Engineering, Changzhou University, Changzhou 213164, China; 2. School of Urban Construction, Changzhou University, Changzhou 213164, China; 3. Taizhou Vocational and Technical College, Taizhou 225300, China
Abstract：This study aimed to develop an electro-catalytic membrane for the efficient removal of pharmaceutical and personal care products (PPCPs) from drinking water. The membrane was fabricated by depositing nanoscale Bi-SnO2 onto carbon membrane (CM) in household water purifiers. To characterized the membranes, scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), and X-ray diffraction (XRD) techniques were employed. The electrochemical performance of the membranes, including oxygen evolution potential, specific capacitance, and impedance, was evaluated using Tafel analysis, cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS). Carbamazepine (CBZ) was chosen as a representative PPCP to assess the electro-catalytic performance of the membranes. The results showed that the particle size of Bi-SnO2 nanoparticles prepared by electrodeposition-hydrothermal method is about 27.2nm, which could be well loaded on the surface of activated carbon filter element, and the electrocatalytic membrane with excellent electrochemical performance was prepared. compared with the base membrane, the Tafel slope increases from 31.09mV/dec to 80.22mV/dec, the electrochemical impedance decreased from 1.03 Ω cm2 to 0.37 Ω cm2, and the specific capacitance increased from 0.689F/g to 2.635F/g. Finally, the degradation effect of carbamazepine was verified by experiments. In the static cycle experiment, the removal rate of CBZ by Bi-SnO2/CM reached 97.3%, the mineralization rate was 59.2% after 1 h, the energy consumption was 123.87kW·h /kgTOC, and ΔTMP was 0.177kPa. In continuous operation, the removal rate of CBZ by Bi-SnO2/CM was 93.7%. The mineralization rate was 35.2%, the energy consumption is 208.33kW·h/kgTOC, and the ΔTMP was 0.613kPa after 1 h. The results showed that the Bi-SnO2/CM electrocatalytic membrane exhibited good electrical conductivity, electrocatalytic activity and stability, and has a good effect on the removal of CBZ.
[1] 樊月婷,昌盛,张坤峰,等.疫情背景下长江中游地区典型饮用水源中PPCPs分布特征与风险评估[J].环境科学, 2022,43(12):5522-5533. Fan Y, Chang S, Zhang K, et al. Distribution characteristics and risk assessment of PPCPs in typical drinking water sources in the middle reaches of the Yangtze River in the context of epidemic[J]. Environmental Science, 2022,43(12):5522-5533. [2] 李牧言,隋倩,黄绍新.上海市典型畜禽养殖场雨水径流中PPCPs的输移特性[J].中国环境科学, 2022,42(8):3643-3649. Li M, Sui Q, Huang S. Transport characteristics of PPCPs in stormwater runoff from typical livestock and poultry farms in Shanghai[J]. China Environmental Science, 2022,42(8):3643-3649. [3] Gao F, He L, Hu L, et al. The variations of antibiotics and antibiotic resistance genes in two subtropical large river basins of South China:Anthropogenic impacts and environmental risks[J]. Environmental pollution (1987), 2022,312:119978. [4] 余绵梓,袁啸,李适宇,等.典型PPCPs在河流沉积物中的吸附特性[J].中国环境科学, 2019,39(4):1724-1733. Yu M, Yuan X, Li S, et al. Adsorption characteristics of typical PPCPs in river sediments[J]. China Environmental Science, 2019,39(4):1724-1733. [5] Timothy Abbott, G.K.C.E. Examination of single-stage anaerobic and anoxic/aerobic and dual-stage anaerobicanoxic/aerobic digestion to remove pharmaceuticals from municipal biosolids[J]. Science of the Total Environment, 2021,791:148237. [6] 陶文嘉.光芬顿陶瓷膜耦合工艺降解卡马西平效能研究[D].北京:北京交通大学, 2020. Tao W. Study on the degradation efficiency of carbamazepine by photoFenton ceramic membrane coupling process[D]. Beijing:Beijing Jiaotong University, 2020. [7] 冯亚丽. Ti/RuO2电极及Pt电极原位生成活性氯降解卡马西平的对比研究[D].武汉:华中科技大学, 2019. Feng Y. Comparative study on in situ generation of active chloro-degradation carbamazepine by Ti/RuO2 electrode and Pt electrode[D]. Wuhan:Huazhong University of Science and Technology, 2019. [8] Wang H, Xi H, Xu L, et al. Ecotoxicological effects, environmental fate and risks of pharmaceutical and personal care products in the water environment:A review[J]. Science of The Total Environment, 2021,788:147819. [9] Ren B, Shi X, Jin X, et al. Comprehensive evaluation of pharmaceuticals and personal care products (PPCPs) in urban sewers:Degradation, intermediate products and environmental risk[J]. Chemical Engineering Journal, 2021,404:127024. [10] Yuan X, Hu J, Li S, et al. Occurrence, fate, and mass balance of selected pharmaceutical and personal care products (PPCPs) in an urbanized river[J]. Environmental pollution (1987), 2020,266:115340. [11] Schapira M, Manor O, Golan N, et al. Involuntary human exposure to carbamazepine:A cross-sectional study of correlates across the lifespan and dietary spectrum[J]. Environment International, 2020,143:105951. [12] 陈爱侠,田铮,卫潇,等.一步法制备磁性多孔碳及高效吸附卡马西平[J].中国环境科学, 2022,42(4):1714-1725. Chen A, Tian Z, Wei X, et al. Preparation of magnetic porous carbon by one-step method and Efficient adsorption of carbamazepine[J]. China Environmental Science, 2022,42(4):1714-1725. [13] 孙继成,吴志超,王志伟,等.电化学耦合膜工艺去除饮用水中卡马西平[J].中国环境科学, 2018,38(1):193-201. Sun J, WU Z, Wang Z, et al. Removal of carbamazepine from drinking water by electrochemical coupled membrane process[J]. China Environmental Science, 2018,38(1):193-201. [14] 吴蕾,彭永臻,李凌云.污水处理厂PPCPs的污染现状与去除技术[J].安全与环境工程, 2021,28(1):179-190. Wu L, Peng Y, LI L. Pollution Status and removal technology of PPCPs in wastewater treatment plant[J]. Safety and Environmental Engineering, 2021,28(1):179-190. [15] 钱虹.电化学协同过硫酸盐氧化水中磺胺类抗生素的试验研究[D].沈阳:沈阳建筑大学, 2018. Qian H. Experimental study on electrochemistry Coordination with persulfate oxidation of sulfonamides in water[D]. Shenyang:Shenyang Jianzhu University, 2018. [16] Fang W, Zhe C, Zhen Z. Construction of visible light responsive ZnO/N-g-C3N4 composite membranes for antibiotics degradation[J]. Journal of Material research and technology, 2022,(17):1696-1706. [17] Du X, Shi Y, Veeriah, et al. A Review on the Mechanism, Impacts and Control Methods of Membrane Fouling in MBR System[J]. Membranes (Basel), 2020,10(2):24. [18] 吴垚,叶俊荣,吴建兴,等.人工湿地去除水中抗生素的研究进展[J].化工技术与开发, 2023,52(3):70-75. Wu Y, Ye J, Wu J et al. Research progress of antibiotic removal from water in constructed wetland[J]. Chemical Technology and Development, 2023,52(3):70-75. [19] Yuan G, Wang Q, Ji G, et al. Degradation of antibiotic pollutants by persulfate activated with various carbon materials[J]. Chemical engineering journal, 2022,429:132387. [20] Li Z, Bao Z, Yao F, et al. One-dimensional bismuth vanadate nanostructures constructed Z-scheme photocatalyst for highly efficient degradation of antibiotics[J]. Journal of Water Process Engineering, 2022,46:102599. [21] Das S, Ahn Y. Synthesis and application of CdS nanorods for LED-based photocatalytic degradation of tetracycline antibiotic[J]. Chemosphere (Oxford), 2022,291(Pt 2):132870-132870. [22] Wang Y,Wu X, Liu J. Mo-modified band structure and enhanced photocatalytic properties of tin oxide quantum dots for visible-light driven degradation of antibiotic contaminants[J]. Journal of environmental chemical engineering, 2022,10(1):107091. [23] Ormeno-Cano N, Radjenovic J. Electrochemical degradation of antibiotics using flow-through graphene sponge electrodes[J]. Journal of hazardous materials, 2022,431:128462. [24] Chao W, Yu G, Chen H, et al. Degradation of norfloxacin by hydroxylamine enhanced fenton system Kinetics, mechanism and degradation pathway[J]. Chemosphere, 2021,270:129408. [25] Estrada-Flórez S, Serna-Galvis E, Torres-Palma R. Photocatalytic vs. sonochemical removal of antibiotics in water:Structure-degradability relationship, mineralization, antimicrobial activity, and matrix effects[J]. Journal of Environmental Chemical Engineering, 2020,8(5):104359. [26] 李雪燕.Bi-SnO2/GO电催化膜的制备及对大肠杆菌去除性能研究[D].天津:天津科技大学, 2020. Li X. Preparation of Bi-SnO2/GO electrocatalytic membrane and its removal performance against Escherichia coli[D]. Tianjin:Tianjin University of Science and Technology, 2020. [27] Rekhate C, Srivastava J. Recent advances in ozone-based advanced oxidation processes for treatment of wastewater-A review[J]. Chemical Engineering Journal Advances, 2020,3:100031. [28] 潘宗林.面向废水处理的煤基导电炭膜设计制备及电化学氧化性能[D].大连:大连理工大学, 2020. Pan Z. Design, preparation and electrochemical oxidation performance of coal-based conductive carbon films for wastewater treatment[D]. Dalian:Dalian University of Technology, 2020. [29] 曲立威,宋海亮,刘燕青,等.电耦合膜生物反应器中膜污染控制的研究进展[J].能源环境保护, 2022,36(4):1-11. Qu L, Song H, Liu Y, et al. Research progress of membrane contamination control in electrically coupled membrane bioreactors[J]. Energy and Environmental Protection, 2022,36(4):1-11. [30] 李玉霞.离心分离-电催化炭膜耦合处理含油废水的研究[D].大连:大连海事大学, 2019. Li Y. Study on the treatment of oily wastewater by centrifugal separation-electrocatalytic carbon membrane coupling[D]. Dalian:Dalian Maritime University, 2019. [31] 王鹏飞.Bi掺杂SnO2电催化炭膜的制备及对大肠杆菌去除性能研究[D].天津:天津科技大学, 2019. Wang P. Preparation of Bi-doped SnO2electrocatalytic carbon film and its removal performance for Escherichia coli[D]. Tianjin:Tianjin University of Science and Technology, 2019. [32] 胡苗,闫共芹,苏一伦,等. In、Bi、Sb掺杂SnO2锂化的第一性原理研究[J].有色金属工程, 2023,13(4):20-28,101. Hu M, Yan C, Su Y, et al. First-principles study on the Litization of SnO2doped with In, Bi and Sb[J]. Nonferrous Metals Engineering, 2023,13(4):20-28,101. [33] 马成龙.铱基催化剂的电化学析氧反应调控机制研究[D].上海:华东理工大学, 2022. Ma C. Study on the regulatory mechanism of electrochemical oxygen evolution reaction of Iridium based catalyst[D]. Shanghai:East China University of Science and Technology, 2022. [34] 张凯.氧化石墨烯改性过渡金属电催化剂的构建及全解水研究[D].无锡:江南大学, 2022. Zhang K. Construction of graphene oxide modified transition metal electrocatalyst and its complete hydrolysis[D]. Wuxi:Jiangnan University, 2022. [35] Anantharaj S, Noda S. How properly are we interpreting the Tafel lines in energy conversion electrocatalysis?[J]. Materials today energy, 2022,29:101123. [36] 解寅珑,云红红,白韡,等.电解水制氢气用催化剂制备及应用性能[J].化学工程师, 2023,37(8):106-111. Xie Y, Yun H, Bai W et al. Preparation and application performance of catalysts for hydrogen production from water electrolysis[J]. Chemical Engineer, 2023,37(8):106-111. [37] 张新奇,朱孟府,邓橙,等. PTFE/Bi-SnO2-CNT电催化膜的结构及性能表征[J].膜科学与技术, 2019,39(1):34-40. Zhang X, Zhu M, Deng C, et al. Characterization of structure and properties of PTFE/Bi-SnO2-CNT electrocatalytic membranes[J]. Membrane Science and Technology, 2019,39(1):34-40. [38] 张新奇.碳纳米管电催化膜的制备及性能研究[D].北京:军事科学院, 2019. Zhang Q,Preparation and properties of carbon nanotube electrocatalyt ic membranes[D]. Beijing:Academy of Military Sciences, 2019. [39] 丁海洋,冯玉杰,刘峻峰.采用循环伏安与Tafel曲线比较不同阳极的电催化性能[J].催化学报, 2007,28(7):646-650. Ding H, Feng Y, Liu J, Comparison of electrocatalytic performance of different anodes by cyclic voltammetry and Tafel curves[J]. Journal of Catalysis, 2007,28(7):646-650. [40] 徐慧敏,赵蕾,何峰,等. Sb-SnO2/OMC电催化膜对水中大肠杆菌的去除效果[J].水处理技术, 2022,48(3):36-39,45. Xu H, Zhao L, He F, et al. Removal effect of Sb-SnO2/OMC electrocatalytic membrane on Escherichia coli in water[J]. Water Treatment Technology, 2022,48(3):36-39,45. [41] 侯志炎.含镍电镀污泥制备超级电容器电极材料及其电化学性能研究[D].乌鲁木齐:新疆大学, 2021. Hou Z. Preparation of electrode materials for supercapacitors from electroplating sludge containing nickel and their electrochemical properties[D]. Urumqi:Xinjiang University, 2021. [42] 李成才.柞木基活性炭的制备及其电化学性能研究[D].大连:大连理工大学, 2021. Li C. Preparation and electrochemical Properties of oak based activated carbon[D]. Dalian:Dalian University of Technology, 2021. [43] 余凌竹.碳基SnO2微纳米球的制备方法及其在扫描电镜校准方面的应用[J].实验科学与技术, 2022,20(1):81-85. Yu L. Preparation of carbon-based SnO2 microspheres and their application in scanning electron microscopy calibration[J]. Experimental Science and Technology, 2022,20(1):81-85. [44] 范影强,陈秀娟,王琳琳,等.水热法制备纳米SnO2电极材料及其储锂性能[J].兰州理工大学学报, 2022,48(5):15-20. Fan Y, Chen X, Wang L et al. Preparation of nano-SnO2 electrode materials by hydrothermal method and their lithium storage properties[J]. Journal of Lanzhou University of Technology, 2022,48(5):15-20. [45] 张慧.SnO2和Bi基催化剂电催化还原CO2至甲酸的研究[D].武汉:华中师范大学, 2014. Zhang H. Study on electrocatalytic reduction of CO2 to formic acid by SnO2 and Bi-based catalysts[D]. Wuhan:Central China Normal University, 2014. [46] Soares A, Tatumi S, Rocca R, et al. Morphological and luminescent properties of HfO2nanoparticles synthesized by precipitation method[J]. Journal of luminescence, 2020,219:116866. [47] 马志浩.菱铁矿催化DTN体系降解水环境中的卡马西平研究[D].哈尔滨:哈尔滨工业大学, 2022. Ma Z. Siderite catalytic degradation of carbamazepine in water environment by DTN system[D]. Harbin:Harbin Institute of Technology, 2022. [48] 冯亚丽.Ti/RuO2电极及Pt电极原位生成活性性氯降解卡马西平的对比研究[D].武汉:华中师范大学, 2019. Feng Y. Comparative study on in situ generation of active chloro-degraded carbamazepine by Ti/RuO2 and Pt electrodes[D]. Wuhan:Central China Normal University, 2019.
