Synergistic enhancement of alkaline hydrogen evolution reaction by role of Ni-Fe LDH introducing frustrated Lewis pairs via vacancy-engineered  

作　　者：Mianfeng Li Haozhi Wang Zijun Yang Zexiang Yin Yuan Liu Yingmei Bian Yang Wang Xuerong Zheng Yida Deng 

机构地区：[1]State Key Laboratory of Marine Resource Utilization in South China Sea,School of Materials Science and Engineering,Hainan University,Haikou 570228,China [2]Tianjin Key Laboratory of Composite and Functional Materials,Key Laboratory of Advanced Ceramics and Machining Technology,(Ministry of Education),School of Materials Science and Engineering,Tianjin University,Tianjin 300072,China

出　　处：《Chinese Chemical Letters》2025年第3期512-516,共5页中国化学快报(英文版)

基　　金：financially supported by National Natural Science Foundation of China(Nos.52301011,52231008,52142304,52177220,U23A200767,52302236,and 22369005);Hainan Provincial Natural Science Foundation of China(Nos.524QN226 and 524QN222);the Key Research and Development Program of Hainan Province(No.ZDYF2022GXJS006);Starting Research Fund from the Hainan University(No.KYQD(ZR)23026);International Science&Technology Cooperation Program of Hainan Province(No.GHYF2023007).

摘　　要：The alkaline hydrogen evolution reaction(HER)is a crucial process for sustainable hydrogen production,yet it requires efficient and stable electrocatalysts to overcome the high activation energy barrier.The article discusses a novel strategy for enhancing the performance of Ni-Fe layered double hydroxide(Ni-Fe LDH)in the alkaline HER by modifying it with a frustrated Lewis acid-base pair(FLP)constructed through vacancy engineering.The study found that the modified Ni-Fe LDH exhibited improved alkaline HER performance.Density functional theory(DFT)calculations demonstrate that the introduction of FLP can activate water and protons more efficiently than monometallic sites,thus reducing the alkaline HER energy barrier and overpotential.In HER under alkaline conditions,the Volmer step involves an additional hydrolysis dissociation compared to acidic conditions,which is one of the factors contributing to the slow reaction kinetics.This paper demonstrates that FLPs can alter the rate-determining step in alkaline HER from the Volmer step to a step with a lower energy barrier,more suitable for hydrogen desorption.The work provides new insights into the role of FLPs in regulating the mechanism and kinetics of HER and opens a new direction for the design and optimization of LDH-based and other electrocatalysts.

关 键 词：Ni-Fe LDH Frustrated Lewis acid-base pair Density functional theory The ab initio molecular dynamics The alkaline hydrogen evolution reaction 

分 类 号：O64[理学—物理化学]