含锡锑中间层的铅锑电极的制备及电催化性能研究

王程程; 李倩; 赵曙光; 宋乐山; 刘画; 张颖; 刘思

doi:10.13205/j.hjgc.202403011

含锡锑中间层的铅锑电极的制备及电催化性能研究

doi: 10.13205/j.hjgc.202403011

深圳永清水务有限责任公司, 广东深圳 518000

基金项目:

永清研发基金项目"三维电催化氧化技术研究"(YQ020821001)

湖南省科技创新重大项目"面向智能制造的自主可控工业互联网关键技术研究与应用示范项目"(2021GK1010)

详细信息

作者简介:
王程程(1987-),女,硕士,工程师,主要从事环境化学、功能材料及水处理技术研究。18229858457@163.com

通讯作者:
赵曙光(1975-),男,博士,教授级高级工程师,主要从事工业水处理及MBR技术的工程应用研究。zsg2509@126.com

计量
- 文章访问数: 76
- HTML全文浏览量: 7
- PDF下载量: 4
- 被引次数: 0
出版历程
- 收稿日期: 2022-12-29
- 网络出版日期: 2024-05-31

PREPARATION AND ELECTRO-CATALYTIC PERFORMANCE OF LEAD-ANTIMONY ELECTRODE WITH A TIN-ANTIMONY INTERMEDIATE LAYER

Shengzhen Yonker Water Co., Ltd., Shenzhen 518000, China

摘要

摘要: 采用溶胶凝胶法制备得到具有高稳定性和高电催化活性的含锡锑中间层的铅锑电极,利用X射线衍射(XRD)、扫描电镜(SEM)、能量色散谱(EDS)、Brunauer-Emmett-Teller(BET)、线性伏安测试(LSV)及循环伏安测试(CV)等测试方法对制备电极的物相结构、表面形貌、元素组成、比表面积及电催化性能进行分析表征,并考察了不同铅锑电极对二(2-乙基己基)磷酸酯废水的电催化降解性能及其稳定性。结果表明:含锡锑中间层的铅锑电极涂层主要为焦绿石型复合氧化物(Pb₃Sb₂O_8.47)_6.4,中间层表面的较大粗糙度及致密结构有利于提高电极稳定性,活性层表面的蜂窝状微孔结构使电催化性能显著增加。LSV及CV测试表明:含锡锑中间层的铅锑电极具有较好的电催化活性及导电性;该电极在电解二(2-乙基己基)磷酸酯废水2 h的COD去除率可达到92.5%,连续使用62 h后COD去除率能维持在91%以上,电极加速寿命可达到30 h,换算成一般工业电流密度(0.1 A/cm²)下的电极实际使用寿命可达到5.5年。含锡锑中间层的铅锑电极具有优越的电催化活性及稳定性,在高盐有机废水处理中具有良好的应用前景。
- 中间层 /
- 铅锑电极 /
- 溶胶凝胶法 /
- 电催化氧化 /
- 稳定性 /
- 二(2-乙基己基)磷酸酯废水
Abstract: In this paper, the lead-antimony electrode with the tin-antimony intermediate layer, with high stability and electrocatalytic activity, was prepared by sol-gel method. The crystal structure, surface morphology, element composition, specific surface area and electrocatalytic performance of the electrode were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), energy-dispersive spectroscopy (EDS), Brunauer-Emmett-Teller(BET), linear sweep voltammetry test(LSV) and cyclic voltammograms test (CV). The electrocatalytic degradation performance and stability of different lead-antimony electrodes were investigated by taking di(2-ethylhexyl) phosphate ester wastewater as the research object. The results indicated that the coating of the lead-antimony electrode with tin-antimony intermediate layer was mainly pyrochlore-type composite oxide, higher roughness and compact structure of the intermediate layer were beneficial to improve the stability of the electrode, and the honeycomb microporous structure of the active layer made electro-catalytic performance significantly increased. The LSV and CV test indicated that the lead-antimony electrode with tin-antimony intermediate layer has better electrocatalytic activity and electrical conductivity, the COD removal rate of the electrode reached 92.5% after 2 hours of electrolysis, and the numerical value could maintain above 91% after 62 hours of continuous operation. The accelerated life of the electrode was up to 30 hours, and its actual life could reach 5.5 years when the accelerated life was converted into the service life, under the condition of the general industrial current density of 0.1 A/cm². The lead-antimony electrode with a tin-antimony intermediate layer has ideal electrocatalytic activity and stability, showing a good application prospect in the treatment of high-salt organic wastewater.
- intermediate layer /
- lead-antimony electrode /
- sol-gel method /
- electrocatalytic oxidation /
- stability /
- di (2-ethylhexyl) phosphate ester wastewater

HTML全文

参考文献(36)

[1]	ASLAN S, SEKERDAG N. Salt inhibition on anaerobic treatment of high salinity wastewater by upflow anaerobic sludge blanket(UASB) reactor[J]. Desalination & Water Treatment, 2016, 57(28):12995-13005.
[2]	焦旭阳,张新妙,栾金义.电催化氧化技术处理含盐有机废水研究进展[J].化工环保, 2019, 39(1):6-8.
[3]	SUNDARAPANDIYAN S, CHANDRASEKAR R, RAMANAIAH B, et al. Electro-chemical oxidation and reuse of tannery saline wastewater[J]. Journal of Hazardous Materials, 2010, 180(1/2/3):197-203.
[4]	徐浩,乔丹,许志成,等.电催化氧化技术在有机废水处理中的应用[J].工业水处理, 2021, 41(3):1-7.
[5]	朱辉,孙文全,孙永军,等.复合负载型γ-Al₂ O₃-Bi-(Sn/Sb)粒子电极电催化降解四环素废水[J].环境工程, 2019,37(1):68-72.
[6]	FENG Y J, LI X Y. Electrochemical degradation of phenol:performance of several metaloxide-based anodes[C]//The 199th Meeting of the Electrochemical Society. Washington DC, USA, 2001.
[7]	ZHU C W, JIANG C Q, CHEN S, et al. Ultrasound enhanced electrochemical oxidation of Alizarin Red S on boron doped diamo-nd (BDD) anode:effect of degradation process parameters[J]. Chemosphere, 2018, 209:685-695.
[8]	ZHENG Y H, SU W Q, CHEN S Y, et al. Ti/SnO₂-Sb₂O₅-RuO₂/α-PbO₂/β-PbO₂ electrodes for pollutants degradation[J]. Chemical Engineering Journal, 2011, 174(1):304-309.
[9]	冯玉杰,沈宏,崔玉虹,等.钛基二氧化铅电催化电极的制备及电催化性能研究[J].分子催化, 2002, 16(3):181-185.
[10]	姚颖悟,周涛,骈岩杰,等.钛基二氧化铅电极的应用与改性研究进展[J].电镀与精饰, 2011, 33(5):17-20.
[11]	吴梦怡,龙昕,高丛浩,等.碳纳米管掺杂PbO₂复合电极的制备及其催化氧化双酚A[J].环境工程, 2021,39(4):51-53.
[12]	XU H, YAN W, YANG H H. Surface analysis of Ti/Sb-SnO₂/PbO₂ electrode after long time electrolysis[J]. Rare Metal Materials and Engineering, 2015, 44 (11):2637-2641.
[13]	AN H, LI Q, TAO D J, et al. The synthesis and characterizaion of Ti/SnO₂-Sb₂O₃/PbO₂ electrodes:the influence of morphology caused by different electrochemical deposition time[J]. Applied Surface Science, 2011, 258 (1):218-224.
[14]	SONG S, ZHAN L Y. Mechanism of the anodic oxidation of 4-chloro-3-methy l phenol in aqueous solution using Ti/SnO₂-Sb/PbO₂ electrodes[J]. Journal of Hazardous Materials, 2010, 175(1/2/3):614-621.
[15]	徐亮,赵芳,农佳莹,等.二氧化铅电极的制备、表征及其电催化性能研究[J].环境工程学报, 2008, 2(7):959-963.
[16]	张惠灵,王晶,彭晓兰,等.不锈钢基PbO₂电极的制备及其降解活性艳兰的研究[J].环境工程, 2009, 27 (4):6-9.
[17]	KONG H S, LU H Y, ZHANG W L, et al. Performance characterization of Ti substrate lead dioxide electrode with different solid solution interlayers[J]. Journal of Material Science, 2012, 47:6709-6715.
[18]	CAO J L, ZHAO H Y, CAO F H, et al. Electrocatalytic degradation of 4-chlorophenol on F doped PbO₂ anodes[J]. Electro-chimica Acta, 2009, 54(9):2595-2602.
[19]	XIA Y J, BIAN X Z, XIA Y, et al. Effect of indium doping on the PbO₂ electrode for the enhanced electrochemical oxidation of aspirin:an electrode comparative study[J]. Separation and Purification Technology, 2020, 237:116-321.
[20]	杨卫华,杨武涛,林小燕.高性能Bi³⁺掺杂改性PbO₂电极的制备及表征[J].物理化学学报, 2012, 28(4):831-836.
[21]	郑辉,戴启洲,王家德,等.La/Ce掺杂钛基二氧化铅电极的制备及电催化性能研究[J].环境科学, 2012, 33(3):858-864.
[22]	沈宏,夏伊静,戴启洲,等.新型二氧化铅电极性能及掺杂机理研究[J].环境科学学报, 2013, 33(2):445-450.
[23]	YAO Y W, JIAO L M, CUI L H, et al. Preparation and characterization of PbO₂-CeO₂ nanocomposite electrode with high cerium content and its application in the electrocatalytic degradation of malachite green[J]. Journal of the Electrochemical Society, 2015, 162 (9):H693-H698.
[24]	环境保护部. 水质化学需氧量的测定重铬酸盐法:HJ 828-2017[S].北京:中国环境出版社,2017.
[25]	韩卫清.电化学氧化法处理难降解有机化工废水的研究[D].南京:南京理工大学, 2007, 32.
[26]	王雅琼,童宏扬,许文林.热分解法制备的Ti/SnO₂+Sb₂O₃/PbO₂电极性质研究[J].无机材料学报,2003,18(5):1033-1038.
[27]	申亚东.蒙脱土基改性催化剂的制备及催化臭氧化效能研究[D].南京:哈尔滨工业大学, 2017, 36-39.
[28]	张开胜,蔡兴国,孔令涛,等.一步法低温合成二维CNx纳米材料及其对水中重金属离子的吸附性能[J].环境工程学报, 2020,14(4):885-887.
[29]	冯玉杰,崔玉虹,王建军.Dy改性SnO₂/Sb电催化电极的制备[J].无机化学学报,2005(10):837-840.
[30]	赵斌,杨阳,邱逢涛,等.不锈钢基Sb-SnO₂/PbO₂电极制备及电沉积因素对其性能影响[J].环境工程, 2023,41(4):26-31 ,39.
[31]	XU M, WANG Z C, WANG F W, et al. Fabrication of cerium doped Ti/nanoTiO₂/PbO₂ electrode with improved electrocatalytic activity and its application in organic degradations[J]. Electrochimica Acta, 2016, 201:240-250.
[32]	王雅琼.含Sb-SnO₂中间层的钛基金属氧化物电极的结构与性能研究[D].南京:南京理工大学, 2008:54-56.
[33]	ZHANG W L, LIN H B, KONG H S, et al. Preparation and characterization of lead dioxide electrode with three-dimensional porous titanium substrate for electrochemical energy storage[J]. Electrochimica Acta, 2014, 139:209-216.
[34]	卢强.涂层钛电极的制备及其降解废水中硝基苯的研究[D].南京:南京理工大学, 2011:34-82.
[35]	FERRERO GA, PREUSS K, MARINOVIC A, et al. Fe-N-doped carbon capsules with outstanding electrochemical performance and stability for the oxygen reduction reaction in both acid and alkaline conditions[J]. ACS Nano, 2016, 10:5922-5929.
[36]	毕强.电化学处理有机废水电极材料的制备与性能研究[D].西安:西安建筑科技大学, 2014:49-55.