文献类型：期刊文献

中文题名：Activating multisite high-entropy alloy nanocrystals via enriching M–pyridinic N–C bonds for superior electrocatalytic hydrogen evolution

英文题名：富M–吡啶N–C键驱动多位点高熵合金纳米晶及其电催化析氢性能

作者：Jingyu Wang[1];Jiahao Zhang[1];Yanjie Hu[1];Hao Jiang[1,2];Chunzhong Li[1,2]

机构：[1]Key Laboratory for Ultrafine Materials of Ministry of Education,Frontiers Science Center for Materiobiology and Dynamic Chemistry,School of Materials Science and Engineering,East China University of Science and Technology,Shanghai 200237,China;[2]Shanghai Engineering Research Center of Hierarchical Nanomaterials,School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China

年份：2022

卷号：67

期号：18

起止页码：1890

中文期刊名：Science Bulletin

外文期刊名：科学通报(英文版)

收录：CSTPCD;;Scopus;CSCD:【CSCD2021_2022】；PubMed;

基金：Acknowledgments This work was supported by the National Natural Science Foun-dation of China (21838003, 51621002) , the Innovation Program ofShanghai Municipal Education Commission, and the Fundamental Research Funds for the Central Universities.

语种：英文

中文关键词：Electrocatalyst;Hydrogen evolution reaction;High-entropy alloy;M–pyridinic N–C;Water splitting

外文关键词：高熵合金;Tafel斜率;电催化剂;配位环境;密度泛函理论计算;原子利用率;电子排布;电流密度;

摘要：The activation of multisite high-entropy alloy(HEA)electrocatalysts is helpful for improving the atomic utilization of each metal in water electrolysis catalysis.Herein,well-dispersed HEA nanocrystals on Nrich graphene with abundant M–pyridinic N–C bonds were synthesized through an ultrasonic-assisted confinement synthesis method.Operando Raman analysis and density functional theory calculations revealed that the electrocatalysts presented the optimal electronic rearrangement with fast ratedetermined H_(2)O dissociation kinetics and favorable H^(*)adsorption behavior that greatly enhanced hydrogen generation in alkaline electrolyte.A small overpotential of only 138.6 mV was required to obtain the current density of 100 mA cm^(-2)and the Tafel slope of as low as 33.0 mV dec^(-1),which was considerably smaller than the overpotentials of the counterpart with poor M–pyridinic N–C bonds(290.4 mV)and commercial Pt/C electrocatalysts(168.6 mV).The atomic structure,coordination environment,and electronic structure were clarified.This work provides a new avenue toward activating HEA as advanced electrocatalysts and promotes the research on HEA for energy-related electrolysis.
激活高熵合金(HEA)电催化剂的多位点是提高金属原子利用率、加速电催化水分解的有效途径.本文采用超声辅助限域合成策略在富氮石墨烯(HNG)载体上成功构筑了尺寸均一、分散均匀的高熵合金纳米晶,并形成了丰富的界面M±吡啶N±C键.原位拉曼分析和密度泛函理论计算结果表明,所制备的HEA/HNG电催化剂表现出最佳的表面电子排布,使其具有快速的水解离动力学和优异的氢吸附行为,显著增强了其碱性析氢性能.HEA/HNG电催化剂仅需138.6 m V的过电势即可达到100 mA cm^(-2)的电流密度,具有低至33.0 m V dec^(-1)的Tafel斜率,优于商用Pt/C电催化剂.本文揭示了高熵合金的原子结构、配位环境和电子结构信息,对设计开发新型高熵合金电催化剂具有重要的指导意义.