Exploring the role of iron in Fe5Ni4S8 toward oxygen evolution through modulation of electronic orbital occupancy

扫码查看

原文链接

NETL
NSTL
万方数据

外文摘要：Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reac-tion(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 liter-ature regarding its role.To clarify this point,we propose a strategy consisting of modulating the elec-tronic 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 tran-sition of Fe5Ni4S8 to highly active catalytic species.The modulated Fe5Ni4S8-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understand-ing the role of Fe in the OER process.

外文关键词：

Oxygen evolutionFe5Ni4S8Electronic orbital occupancy modulationReconstruction dynamics

作者：

Zhengyan Du、Zeshuo Meng、Haoteng Sun、Yifan Li、Chao Jiang、Yaxin Li、Xiaoying Hu、Yi Cui、Shansheng Yu、Hongwei Tian

展开 >

作者单位：

Key Laboratory of Automobile Materials of MOE,School of Materials Science and Engineering,Jilin University,Changchun 130012,Jilin,China

Department of Chemistry,Brown University,RI 02912,United States

i-lab,Vacuum Interconnected Nanotech Workstation(Nano-X),Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences,Suzhou 215123,Jiangsu,China

College of Science and Laboratory of Materials Design and Quantum Simulation,Changchun University,Changchun 130022,Jilin,China

展开 >

基金：

Scientific and Technological Development Program of Jilin ProvinceNational Key R&D Program of ChinaCAS Project for Young Scientists in Basic ResearchYoung Cross Team Project of CAS

项目编号：

20220201138GX2022YFA1503801YSBR-022JCTD-2021-14

出版年：

2024

DOI：

10.1016/j.jechem.2024.01.028

能源化学

中国科学院大连化学物理研究所中国科学院成都有机化学研究所

能源化学

CSTPCDEI

影响因子：0.654

ISSN：2095-4956

年,卷(期)：2024.92(5)