Reversible Structural Oscillation Mediates Stable Oxygen Evolution Reaction
Abstract
Abstract The dynamic dissolution of active species of electrocatalysts suffers severe durability issues, thus limiting practical sustainable electrochemical application despite the enormous strides in the activity. An atomistic understanding of the dynamic pattern is a fundamental prerequisite for realizing prolonged stability. Herein, modeling on NiFe LDHs, multiple operando spectroscopies revealed the structural oscillation of the local [Ni–O 2 –Fe] unit identified a strong dependence on the alternant Fe dissolution and redeposition during the oxygen evolution reaction (OER) process, thus mediating the dynamic stability. At this point, a proof‐of‐concept strategy with S, Co co‐doping was demonstrated to tune structural oscillations. In situ S leaching that alleviates the lattice mismatch suppresses Fe dissolution, while the electron‐withdrawing Co as a deposition site promotes Fe redeposition, thus achieving the reversible oscillation of local [Ni/Co–O 2 –Fe] units and dynamic stability. The implementation of the modified NiFe LDH in industrial water electrolysis equipment operated steadily over 800 h (5000‐h lifetime obtained by epitaxial method with 10% attenuation) with an energy consumption of 4.05 kWh Nm −3 H 2 @ 4000 A m −2 . The levelized cost of hydrogen of US$ 2.315 per kg H2 overmatches the European Commission's target for the coming decade (<US$ 2.5 per kg H2 ).
Article Details
Authors (13)
Qunlei Wen
State Key Laboratory of Advanced Electromagnetic Technology, School of Electrical and Electronic Engineering, Huazhong University of Science and Technology
Tianyang Liu
Jiangsu Co-Innovation Centre of Efficient Processing and Utilization of Forest Resources, College of Chemical Engineering
Danji Huang
State Key Laboratory of Advanced Electromagnetic Technology, School of Electrical and Electronic Engineering, Huazhong University of Science and Technology
Yu Lin
Zhenhong Yang
State Key Laboratory of Advanced Electromagnetic Technology, School of Electrical and Electronic Engineering, Huazhong University of Science and Technology
Ruoou Yang
State Key Laboratory of Materials Processing and Die & Mould Technology, and School of Materials Science and Engineering
Youwen Liu
State Key Laboratory of Materials Processing and Die & Mould Technology, and School of Materials Science and Engineering
Xiaomeng Ai
State Key Laboratory of Advanced Electromagnetic Technology, School of Electrical and Electronic Engineering, Huazhong University of Science and Technology
Jiakun Fang
State Key Laboratory of Advanced Electromagnetic Technology, School of Electrical and Electronic Engineering, Huazhong University of Science and Technology
Yafei Li
Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, School of Chemistry and Materials Science
Bao Yu Xia
State Key Laboratory of New Textile Materials and Advanced Processing, Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering
Shijie Cheng
Tianyou Zhai
State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering