Boosting Electrocatalytic Oxygen Evolution by Cation Defect Modulation via Electrochemical Etching  

作　　者：Xiang Chen Meng Yu Zhenhua Yan Weiyi Guo Guilan Fan Youxuan Ni Jiuding Liu Wei Zhang Wei Xie Fangyi Cheng Jun Chen 

机构地区：[1]Renewable Energy Conversion and Storage Center,Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Engineering Research Center of High-efficiency Energy Storage(Ministry of Education),College of Chemistry,Nankai University,Tianjin 300071

出　　处：《CCS Chemistry》2021年第1期675-685,共11页中国化学会会刊（英文）

基　　金：supported by MOST(2017YFA0206700 and 2018YFB1502100);NSFC(21871149,21925503,and 51571125);MOE(B12015);Tianjin Project(18JCZDJC31100);the Fundamental Research Funds for the Central Universities.

摘　　要：Defects engineering is an efficient strategy to enhance the performance of electrode materials by modulating the local electronic structure but usually requires costly and complicated processing.Here,an electrochemical reduction etching method has been developed for controllable tailoring of the cationic defects in iron-based oxides under mild conditions.The optimized defective spinel-type iron nickel oxide exhibits an overpotential as low as 270 mV at 10 mA cm−2 and a Tafel slope of only 33.8 mV dec−1 for the oxygen evolution reaction(OER),outperforming the benchmark RuO2 and pristine oxide.Experiments and theoretical calculations reveal that Fe vacancies can enhance Ni–O covalency,increase the density of active sites,and optimize the surface electronic structure,which promote the water adsorption/activation and moderate oxygen intermediate species adsorption,thus significantly enhancing OER activity.This work provides a promising approach to create cation deficiency and mechanistic insight to understand the vacancy-induced enhancement of oxygen electrocatalysis.

关 键 词：defect chemistry electrochemical synthesis spinel oxide oxygen evolution metal–oxygen covalency 

分 类 号：O64[理学—物理化学]