复合负载型γ-Al_2O_3-Bi-(Sn/Sb)粒子电极电催化降解四环素废水
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摘要
以模拟废水中的四环素(TC)和TOC(总有机碳)去除率为研究指标,探讨粒子电极的不同体系对降解四环素废水的影响。同时以浸渍法优化制备不同负载型γ-Al_2O_3粒子电极,并研究了其电催化性能和降解能耗,考察浸渍法和后浸渍法制备粒子电极的优劣。结果表明:三维电解体系对TC的降解效果达到40.1%,明显优于二维体系的29.1%;不同负载型粒子电极对TC的降解效果依次为Bi>Sn/Sb>Ti>Co>Cu>Fe>Mn,其中γ-Al_2O_3-Bi粒子电极对TC和TOC的去除效果最佳,分别为63.8%、36.3%;γ-Al_2O_3-Bi和γ-Al_2O_3-Sn/Sb粒子电极的能耗分别为85.9,90.7 (kW·h)/kg,远低于二维降解体系(205.5 (kW·h)/kg);浸渍法制得的γ-Al_2O_3-Bi-(Sn/Sb)对TC的电解效率明显优于后浸渍法制得的粒子电极,其中前者为78.9%,高出后者约10百分点。
The effects of different systems of particle electrodes on the degradation of tetracycline wastewater were studied based the removal rate of TC(tetracycline) and TOC(total organic carbon) in simulated wastewater as the research indexes. Simultaneously, different supported γ-Al_2O_3 particle electrodes were optimized and prepared by impregnation method, and their electro-catalytic properties and degradation energy consumption were investigated, and finally, the advantages and disadvantages of impregnation method and post-impregnation method in preparing particle electrodes were studied. The experimental results showed that the degradation effect of TC by the three-dimensional electrolysis system reached 40.1%, which was obviously better than 29.1% of the two-dimensional electrolysis system; the TC degradation effect by different supported particle electrodes was in order of Bi> Sn/Sb> Ti> Co> Cu> Fe> Mn, with γ-Al_2O_3-Bi particle electrodes having the best removal effect of TC and TOC, which were 63.8% and 36.3%, respectively; the energy consumptions of the γ-Al_2O_3-Bi and γ-Al_2O_3-Sn/Sb particle electrolysis were 85.9(kW·h)/kg and 90.7(kW·h)/kg respectively, which were far below that of the two-dimensional degradation system(205.5(kW·h)/kg); in addition, the electrolysis efficiency of γ-Al_2O_3-Bi-(Sn/Sb) particles prepared by impregnation method was obviously better than that by the post-impregnation method, with the former(78.9%) being about 10% higher than the latter.
The effects of different systems of particle electrodes on the degradation of tetracycline wastewater were studied based the removal rate of TC(tetracycline) and TOC(total organic carbon) in simulated wastewater as the research indexes. Simultaneously, different supported γ-Al_2O_3 particle electrodes were optimized and prepared by impregnation method, and their electro-catalytic properties and degradation energy consumption were investigated, and finally, the advantages and disadvantages of impregnation method and post-impregnation method in preparing particle electrodes were studied. The experimental results showed that the degradation effect of TC by the three-dimensional electrolysis system reached 40.1%, which was obviously better than 29.1% of the two-dimensional electrolysis system; the TC degradation effect by different supported particle electrodes was in order of Bi> Sn/Sb> Ti> Co> Cu> Fe> Mn, with γ-Al_2O_3-Bi particle electrodes having the best removal effect of TC and TOC, which were 63.8% and 36.3%, respectively; the energy consumptions of the γ-Al_2O_3-Bi and γ-Al_2O_3-Sn/Sb particle electrolysis were 85.9(kW·h)/kg and 90.7(kW·h)/kg respectively, which were far below that of the two-dimensional degradation system(205.5(kW·h)/kg); in addition, the electrolysis efficiency of γ-Al_2O_3-Bi-(Sn/Sb) particles prepared by impregnation method was obviously better than that by the post-impregnation method, with the former(78.9%) being about 10% higher than the latter.
引文
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[3] Snyder S A, Westerhoff P, Yoon Y, et al. Personal care products, and endocrine disruptors in water: implications for the water industry[J]. Environmental Engineering Science, 2003, 20(13): 449-469.
[4] Xu W H, Zhang G, Zou S C, et al. Determination of selected antibiotice in the Cictoria Harbour and the Pearl River, South China using high-performance liquid chromatography-electrospray ionization tandem mass spectrometry[J]. Environmental Pollution, 2007, 145(3): 672-679.
[5] 欧丹云, 陈彬, 陈灿祥, 等. 九龙江下游河口水域抗生素及抗性细菌的分布[J]. 中国环境科学, 2013, 33(12): 2243-2250.
[6] Elmolla E S, Chaudhuri M. Feasibility of using combined TiO2 photocatalysis-SBR process for antibiotic wastewater treatment[J]. Desalination, 2011,272(1): 218-224.
[7] Zhang J C, Giorno L, Drioli E. Study of a hybrid process combining PACs and membrane operations for antibiotic wastewater treatment[J]. Desalination, 2006, 194(1): 101-107.
[8] 赵文杰, 孙雪菲, 丁可, 等. 一种新型改性交联壳聚糖的制备及其对废水中四环素的去除机理[J]. 山东大学学报(工学版), 2014, 44(5): 65-71.
[9] Cazes M D, Belleville M P, Petit E, et al. Design and optimization of an enzymatic membrane reactor for tetracycline degradation[J]. Catalysis Today, 2014, 236(11): 146-152.
[10] 张岩, 高明明, 王新华, 等. 光电Fenton耦合转盘技术处理四环素废水[J]. 环境化学, 2016, 35(5): 893-900.
[11] 丁杰, 宋昭, 宋迪慧,等. 三维电催化处理苯并噻唑反应器结构优化[J]. 化工进展, 2017, 36(1):91-99.
[12] 王美莲, 朱学武, 成小翔,等. 饮用水电化学和膜分离除氟技术发展与展望[J]. 给水排水, 2017(11):112-122.
[13] Botte G G, Botte G G. Electrochemical technologies for water treatment, management, and efficiency[J]. Electrochemical Society Interface, 2017, 26(2):53-61.
[14] Sun W Q, Ma G C, Sun Y J, et al. Effect treatment of high phosphorus Pharmaceutical wastewater by chemical precipitation[J]. The Canadian Journal of Chenical Engineering, 2017, 95(8): 1585-1593.
[15] 汤佳伟, 孙文全, 孙永军, 等. Ti-Ni/γ-Al2O3粒子电极的制备及其处理氯霉素废水的效果[J]. 环境污染与防治, 2017, 39 (11): 1177-1180.
[16] Dias R M B, Vieira A J S C. Effect of oxygen on the hydroxylation of adenine by photolytically generated hydroxyl radical[J]. Journal of Photochemistry & Photobiology A Chemistry, 1997, 109(2): 133-136.
[17] 徐海青, 刘秀宁, 王育乔, 等. 复合金属氧化物Sn-Sb-Mn/陶瓷粒子电极体系的电催化性能[J]. 物理化学学报, 2009, 25 (5): 840-846.
[18] Wang X, Pan X, Lin R, et al. Steam reforming of dimethyl ether over Cu-Ni/γ-Al2O3 bi-functional catalyst prepared by deposition-precipitation method[J]. International Journal of Hydrogen Energy, 2010, 35(9): 4060-4068.
[19] Wang X L, Pan X M, Lin R, et al. Dimethyl ether steam reforming for hydrogen production over Cu-Ni/γ-Al2O3 Bi-functional catalyst[J]. Acta Physico-Chimica Sinica, 2010, 25(6): 1296-1304.
[20] 王宁, 孙自瑾, 王永钊, 等. Ni-Fe/γ-Al2O3双金属催化剂的制备及其CO甲烷化性能研究[J]. 燃料化学学报, 2011, 39(3): 219-223.
[21] Cui X, Zhao G, Lei Y, et al. Novel vertically aligned TiO2 nanotubes embedded with Sb-doped SnO2 electrode with high oxygen evolution potential and long service time[J]. Materials Chemistry & Physics, 2009, 113(1): 314-321.
[22] Santana M H P, Faria L A D, Boodts J F C. Electrochemical characterisation and oxygen evolution at a heavily boron doped diamond electrode[J]. Electrochimica Acta, 2005, 50(10): 2017-2027.
[23] 刘世永, 王宇新, 许莉. 降低水电解中阳极析氧过电位的研究进展[J]. 电池, 2006(2): 74-75.
[24] 张郸宁. 新型镍基催化剂的制备及其对苯酚的加氢应用[D]. 郑州:郑州大学,2016.
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