摘要
Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction due to thermodynamic instability,which has resulted in conflicting reports within the literature regarding its role.To clarify this point,we propose a strategy consisting of modulating the electronic orbital occupancy to suppress the extensive loss of Fe atoms during the OER process.Theoretical calculations,in-situ X-ray photoelectron spectroscopy,molecular dynamics simulations,and a series of characterization showed that the stable presence of Fe not only accelerates the electron transfer process but also optimizes the reaction barriers of the oxygen evolution intermediates,promoting the phase transition of Fe_(5)Ni_(4)S_(8)to highly active catalytic species.The modulated Fe_(5)Ni_(4)S_(8)-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understanding the role of Fe in the OER process.
基金
financially supported by the Scientific and Technological Development Program of Jilin Province(20220201138GX)
the support of the National Key R&D Program of China(No.2022YFA1503801)
CAS Project for Young Scientists in Basic Research(No.YSBR-022)
the Young Cross Team Project of CAS(No.JCTD-2021-14)。
作者简介
Corresponding author:Xiaoying Hu,E-mail addresses:huxy@ccu.edu.cn;Corresponding author:Yi Cui,ycui2015@sinano.ac.cn;Corresponding author:Shansheng Yua,yuss@jlu.edu.cn;Corresponding author:Hongwei Tian,tianhw@jlu.edu.cn;These authors contributed equally to this work:Zhengyan Du;These authors contributed equally to this work:Zeshuo Meng。
