宋贺庆,杨海涛,俞小花,胡超权

• 1:昆明理工大学冶金与能源工程学院
• 2:中国科学院过程工程研究所
• 3:中科南京绿色制造产业创新研究院

摘要(Abstract)：

以Ti/Nb的质量比为100、75、50、25和10配制了中间层溶液，以原子比Ir∶Ru∶Ti=1∶3∶3配制了活性层溶液，采用热分解法制备了钛基铌-钛中间层的涂层电极。对其在酸性析氧条件下的改性性能进行研究，并分析其失效机理。利用X射线衍射(XRD)、扫描电镜(SEM)和能谱仪(EDS)分析其失效前后的物相和形貌变化，通过强化电解寿命实验、电化学分析等研究了RuO_2-IrO_2-TiO_2/NbO_x-TiO_2/Ti电极在酸性体系中的性能。结果表明：在酸性体系下，电极失效主要是由活性层的溶解脱落以及电极表面生成不导电的钛氧化物造成的；中间层铌-钛比为1∶10的涂层电极寿命更佳，较未掺杂中间层的涂层阳极寿命提升明显，但电压增加；综合考虑能耗与服役时间，中间层铌-钛比为1∶25的电极更符合实际生产的需求。

关键词(KeyWords)： 钛涂层电极;铌-钛中间层;电化学性能;强化电解寿命

Abstract:

Keywords:

基金项目(Foundation): 国家自然科学基金(22078328,51504231);; 多相复杂系统国家重点实验室(MPCS-2022-A-02);; 中国科学院绿色过程制造创新研究院(IAGM2022D08);; 云南省万人计划项目(YNWR-QNBJ-2018-327)

作者(Author): 宋贺庆,杨海涛,俞小花,胡超权

DOI: 10.13289/j.issn.1009-6264.2023-0579

参考文献(References)：

• [1] Denton D A,Harrison J A,Knowles R I.Automation of electrode kinetics—IV.The chlorine evolution reaction on a RuO2-TiO2 plate electrode[J].Electrochimica Acta,1980,25:1147-1152.
• [2] Vasudevan S.Effect of cations of alkali and alkaline-earth metal chlorides for chlorine evolution reaction[J].Industrial Engineering Chemistry Research,2008,47(3):976-979.
• [3] Karlsson R K B,Cornell A.Selectivity between oxygen and chlorine evolution in the chlor-alkali and chlorate processes[J].Chemical Reviews,2016,116(5):2982-3028.
• [4] Xiong K,Deng Z,Li L,et al.Sn and Sb co-doped RuTi oxides supported on TiO2 nanotubes anode for selectivity toward electrocatalytic chlorine evolution[J].Journal of Applied Electrochemistry,2013,43(8):847-854.
• [5] 姚立广，王明贤.析氯钛基RuO2-Co3O4-TiO2(60)涂层的研究[J].电化学，1996,2(3):285-293.YAO Li-guang,WANG Ming-xian.A study of RuO2-Co3O4-TiO2(60) coating on Ti-substrate for chlorine gas evolution[J].Electrochemistry,1996,2(3):285-293.
• [6] 赵小云，王三反，周键，等.Ce含量对Ti/IrO2-SiO2-CeO2电极电催化性能的影响[J].有色金属工程，2019,9(12):22-28.ZHAO Xiao-yun,WANG San-fan,ZHOU Jian,et al.Effect of Ce content on electrocatalytic performance of Ti/IrO2-SiO2-CeO2 electrode[J].Nonferrous Metals Engineering,2019,9(12):22-28.
• [7] 刘新辉.涂层钛电极在高盐有机废水处理中的原理和应用[J].化工管理，2021(27):42-43.LIU Xin-hui.Principle and application of coated titanium electrode in treatment of high salt organic wastewater[J].Chemical Engineering Management,2021(27):42-43.
• [8] 俞胜三，李乐卓，王三反.DSA电极的改性及其在有机废水处理中的研究进展[J].应用化工，2022,51(8):2406-2409.YU Sheng-san,LI Le-zhuo,WANG San-fan.Modification of DSA electrode and its research progress in organic wastewater treatment[J].Applied Chemical Industry,2022,51(8):2406-2409.
• [9] 迟明超，运晓静，罗斌，等.DSA电极的制备及应用的研究进展[J].应用化工，2021,50(2):498-503.CHI Ming-chao,YUN Xiao-jing,LUO Bin,et al.Research progress on preparation and application of DSA electrode[J].Applied Chemical Industry,2021,50(2):498-503.
• [10] 徐永海，罗小军，张招贤.阴极保护用涂层钛电极(一)[J].电镀与涂饰，2011,30(4):50-55.XU Yong-hai,LUO Xiao-jun,ZHANG Zhao-xian,et al.Coated titaniumelectrodes used for cathodicprotection—Part I[J].Electroplating & Finishing,2011,30(4):50-55.
• [11] 胡媛媛.TiCl4水解法制备高催化活性析氯钛阳极及其性能研究[J].材料保护，2020,53(7):46-48.HU Yuan-yuan.Preparation and performance of titanium anode with high catalytic activity forchloride evolution by TiCl4 hydrolysis method[J].Material Protection,2020,53(7):46-48.
• [12] Moradi F,Dehghanian C.Addition of IrO2 to RuO2+TiO2 coated anodes and its effect on electrochemical performance of anodes in acid media[J].Progress in Natural Science:Materials International,2014,24(2):134-141.
• [13] 李茂梅，许林成，白帆，等.复合材料Fe0.5Co0.25Ni0.25Ox-Ti4O7电极的制备及催化活性研究[J].有色金属工程，2020,10(2):16-21.LI Mao-mei,XU Lin-cheng,BAI Fan,et al.Preparation and catalytic activity of composite Fe0.5Co0.25Ni0.25Ox-Ti4O7 electrode[J].Nonferrous Metals Engineering,2020,10(2):16-21.
• [14] 曹迪，曹敏，孙宁磊，等.钌铱及铱钽氧化物涂层钛电极加速寿命及失效原因研究[J].绿色矿冶，2023,39(2):34-38.CAO Di,CAO Min,SUN Ning-lei,et al.Study on the accelerated life and failure analysis of ruthenium-iridium oxides and iridium-tantalum oxides coated titanium electrodes[J].Sustainable Mining and Metallurgy,2023,39(2):34-38.
• [15] 戴红，徐杉，黄焱，等.钛基钌系氧化物涂层阳极电催化水处理活性与失活[J].贵金属，2019,40(3):70-75.DAI Hong,XU Shan,HUANG Yan,et al.Activation and deactivation of titanium-based rutheniumoxide coating anode in electrocatalysis water treatment[J].Precious Metals,2019,40(3):70-75.
• [16] 陈永毅，王欣，邵艳群，等.Ru-Ti和Ir-Ta不同组合涂层钛阳极的组织形貌[J].中国有色金属学报，2009,19(4):689-694.CHEN Yong-yi,WANG Xin,SHAO Yan-qun,et al.Structure and morphology of titanium anode coating withdifferent combinations from Ru-Ti and Ir-Ta[J].The Chinese Journal of Nonferrous Metals,2009,19(4):689-694.
• [17] 赵瑞玉，王艺谋，赵会吉，等.Ti/SnO2涂层电极的制备研究进展[J].应用化工，2022,51(8):2348-2354.ZHAO Rui-yu,WANG Yi-mou,ZHAO Hui-ji,et al.Progress in the preparation of Ti/SnO2 coated electrodes[J].Applied Chemical Industry,2022,51(8):2348-2354.
• [18] 俞益航，王新令，励蓉，等.基于TNTs中间层的钌铱钽氧化物阳极制备及强化寿命研究[J].表面技术，2022,51(2):384-391.YU Yi-hang,WANG Xin-ling,LI Rong,et al.Preparation and accelerating life testing of RuIrTa oxide anode with TNTs interlayer[J].Surface Technology,2022,51(2):384-391.
• [19] 胡杰珍，邓培昌，徐海波，等.铱钛氧化物中间层对钛基氧化铱电极组织及析氧行为的影响[J].电镀与涂饰，2010,29(4):66-69.HU Jie-zhen,DENG Pei-chang,XU Hai-bo,et al.Effect of iridium-titanium oxide interlayer on the microstructure and oxygen evolution behavior of Ti/IrO2-coated electrode[J].Electroplating & Finishing,2010,29(4):66-69.
• [20] 杨森，王雁，李乐琰，等.Ir对TiO2-RuO2涂层钛电极析氯性能的影响[J].电镀与涂饰，2023,42(16):23-32.YANG Sen,WANG Yan,LI Le-yan,et al.Effect of iridium on chlorine evolution performance of titanium-ruthenium oxide electrode[J].Electroplating & Finishing,2023,42(16):23-32.
• [21] 朱君秋，王欣，路恒达，等.钛基RuO2-Ta2O5涂层电极材料的电容性能分析[J].材料热处理学报，2012,33(7):122-126.ZHU Jun-qiu,WANG Xin,LU Heng-da,et al.Preparation and capacitance performance of Ti/RuO2-Ta2O5 electrodes[J].Transactions of Materials and Heat Treatment,2012,33(7):122-126.
• [22] 赵国军.基于TNTs中间层的钌钛复合电极的制备及性能研究[D].杭州：浙江工业大学，2020.ZHAO Guo-jun.Preparation and properties of Ru-Ti composite electrode based on TNTs interlayer[D].Hangzhou:Zhejiang University of Technology,2020.
• [23] 景海龙，杨泽坤，杨海涛，等.Ti/RuO2-IrO2阳极在碱性体系的失效行为[J].有色金属工程，2023,13(3):23-30.JING Hai-long,YANG Ze-kun,YANG Hai-tao,et al.Failure behavior of Ti/RuO2-IrO2 anodes in alkaline systems[J].Nonferrous Metals Engineering,2023,13(3):23-30.
• [24] Dou Q,Shrotriya P,Li W,et al.Stress-generating electrochemical reactions during the initial growth of anodic titanium dioxide nanotube layers[J].Electrochimica Acta,2019,295:418-426.
• [25] Hu J M,Zhang J Q,Meng H M,et al.Microstructure,electrochemical surface and electrocatalytic properties of IrO2+Ta2O5 oxide electrodes[J].Journal of Materials Science,2003,38(4):705-712.
• [26] 吴维兰.含钽中间层钛基金属氧化物电极的性能研究[D].济南：山东大学，2011.WU Wei-lan.Study on titanium-based metal oxide anode with tantalum interlayer coating[D].Jinan:Shandong University,2011.

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