Electro‑copolymerized film of ruthenium catalyst and redox mediator for electrocatalytic water oxidation  

基于钌催化剂和电子转移介质电化学共聚膜的电催化水氧化

作　　者：WANG Hao TANG Kun SHAO Jiangyang WANG Kezhi ZHONG Yuwu 王浩;唐坤;邵将洋;王克志;钟羽武(中国科学院化学研究所,北京分子科学国家研究中心,中国科学院光化学重点实验室,中国科学院分子科学科教融合卓越创新中心,北京100190;北京师范大学化学学院,能量转换与存储材料北京市重点实验室,北京100875;中国科学院大学化学科学学院,北京100049)

机构地区：[1]Beijing National Laboratory for Molecular Sciences,CAS Research/Education Center for Excellence in Molecular Sciences,Key Laboratory of Photochemistry,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China [2]Beijing Key Laboratory of Energy Conversion and Storage Materials,College of Chemistry,Beijing Normal University,Beijing 100875,China [3]School of Chemical Sciences,University of Chinese Academy of Sciences,Beijing 100049,China

出　　处：《无机化学学报》2024年第11期2193-2202,共10页Chinese Journal of Inorganic Chemistry

基　　金：国家自然科学基金(No.21925112,21975264,22090021);中国科学院青年创新促进会基金资助。

摘　　要：Electro-copolymerized film containing ruthenium complexes as electron-transfer(or redox)mediators and water-oxidation catalysts by an oxidative copolymerization method is presented.The addition of the redox mediator significantly improved the electrocatalytic water-oxidation activity and reduced the overpotential to 220 mV.The prepared electrode showed a water-oxidation catalytic rate constant kobs of 31.7 s^(-1)and an initial turnover frequency of 1.01 s^(-1)in 1000 s by potential electrolysis at 1.7 V applied bias vs NHE(normal hydrogen electrode).The kinetic isotope effect study suggests that the catalytic water oxidation reaction on the electrode surface occurs via a bimolecular coupling mechanism.本文介绍了一种钌催化剂和电子转移介质共聚的氧化电聚合薄膜的制备及其在电催化水氧化中的应用。电子转移介质的引入显著提高了钌催化剂的电催化水氧化活性,并将过电位降低到了220 mV。所制备的电聚合电极的水氧化催化速率常数kobs为31.7 s^(-1),在1.7 V偏压下电解1000 s后的转换频率为1.01 s^(-1)。同位素动力学结果表明,电极表面的催化水氧化反应主要通过双分子耦合机理进行。

关 键 词：water oxidation water splitting ruthenium complexes ELECTROPOLYMERIZATION ELECTROCATALYSIS 

分 类 号：O614.821[理学—无机化学]