文献类型：期刊文献

英文题名：A new operando surface restructuring pathway via ion-pairing of catalyst and electrolyte for water oxidation

作者：Zhuang, Linzhou[1,2];Li, Zhiheng[2];Li, Mengran[2,3];Tao, Haolan[1];Mao, Xin[4];Lian, Cheng[1];Ge, Lei[5];Du, Aijun[4];Xu, Zhi[1];Shao, Zongping[6,7];Zhu, Zhonghua[2]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Univ Queensland, Sch Chem Engn, Brisbane 4072, Australia;[3]Delft Univ Technol, Fac Appl Sci, Dept Chem Engn, Maasweg 9, NL-2629 HZ Delft, Netherlands;[4]Queensland Univ Technol, Ctr Mat Sci, George St, Brisbane 4001, Australia;[5]Univ Southern Queensland, Ctr Future Mat, Springfield Cent, Toowoomba, Qld 4300, Australia;[6]Curtin Univ Technol, Dept Chem Engn, Perth, WA 6845, Australia;[7]Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 211816, Peoples R China

年份：2023

卷号：454

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20224413052237);WOS:【SCI-EXPANDED(收录号:WOS:000915924700003)】；

基金：L. Z. and Z. L. contributed equally to this work. Z. Z. likes to thank the financial support from Australian Research Council Discovery Projects (DP190101782) and (DP200101397) . The authors thank the valuable advice from Prof. Honglai Liu about the DFT calculation. The authors also thank the Shanghai Synchrotron Radiation Facility (BL14W1, SSRF) for XAS equipment access.

语种：英文

外文关键词：Operando surface restructuring; Strontium ion leaching; Cation size -matching; Oxygen evolution; Non -acidic medium

摘要：The highly efficient and stable electrolysis needs the rational control of the catalytically active interface during the reactions. Here we report a new operando surface restructuring pathway activated by pairing catalyst and electrolyte ions. Using SrCoO3-delta-based perovskites as model catalysts, we unveil the critical role of matching the catalyst properties with the electrolyte conditions in modulating catalyst ion leaching and steering surface restructuring processes toward efficient oxygen evolution reaction catalysis in both pH-neutral and alkaline electrolytes. Our results regarding multiple perovskites show that the catalyst ion leaching is controlled by catalyst ion solubility and anions of the electrolyte. Only when the electrolyte cations are smaller than catalyst's leaching cations, the formation of an outer amorphous shell can be triggered via backfilling electrolyte cations into the cationic vacancy at the catalyst surface under electrochemical polarization. Consequently, the current density of reconstructed SrCoO3-delta is increased by 21 folds compared to the pristine SrCoO3-delta at 1.75 V vs reversible hydrogen electrode and outperforms the benchmark IrO2 by 2.1 folds and most state-of-the-art electrocatalysts in the pH-neutral electrolyte. Our work could be a starting point to rationally control the electrocatalyst surface restructuring via matching the compositional chemistry of the catalyst with the electrolyte properties.