Bimetallic carbide electrocatalysts have great potential to outperform well-defined single metal ones for the electrochemical hydrogen evolution reaction(HER).However,the lack of regulation tactics of electronic struc...Bimetallic carbide electrocatalysts have great potential to outperform well-defined single metal ones for the electrochemical hydrogen evolution reaction(HER).However,the lack of regulation tactics of electronic structures largely impedes the upgrading of bimetallic carbides for efficient hydrogen evolution.Herein,a novel Ni_(3)ZnC_(0.7)/Ni heterostructure embedded in N-doped carbon nanotubes(Ni_(3)ZnC_(0.7)/Ni@CNTs)was synthesized by a facile one-step pyrolysis protocol.Experimental and theoretical results demonstrated that the electronic coupling interaction between Ni and Ni_(3)ZnC_(0.7) triggered the redistribution of interfacial charge and optimized the electronic state density of metallic Ni sites,which reduced the H^(*) adsorption–desorption energy barrier and thus accelerated the HER kinetics in the electrocatalytic process.The resulting Ni_(3)ZnC_(0.7)/Ni@CNTs required ultralow overpotentials of 93 and 256 mV to deliver current densities of 10 and 100 mA cm^(−2) for the HER,respectively,and exhibited extraordinary long-term durability for at least 400 h in 1.0 M KOH solution.This work provides a novel perspective for the design of high-performance bimetallic carbide electrocatalysts for water splitting.展开更多
基金supported by the National Natural Science Foundation of China(No.22179074,U22A20144,52073166 and 52172049)the Program for International S&T Cooperation Projects of Shaanxi Province(2020GHJD-04 and 2023GHZD-08)+4 种基金the Scientific Research Project of Education Department of Shaanxi Province(No.22JK0297)the Doctoral Scientific Research Startup Foundation of Shaanxi University of Science and Technology(2016QNBT-07)the Open Foundation of Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and Technology(No.KFKT2023-01)Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry and Technology,Shaanxi University of Science and Technology(No.KFKT2023-01)the Young Talent Fund of Xi’an Association for Science and Technology.
文摘Bimetallic carbide electrocatalysts have great potential to outperform well-defined single metal ones for the electrochemical hydrogen evolution reaction(HER).However,the lack of regulation tactics of electronic structures largely impedes the upgrading of bimetallic carbides for efficient hydrogen evolution.Herein,a novel Ni_(3)ZnC_(0.7)/Ni heterostructure embedded in N-doped carbon nanotubes(Ni_(3)ZnC_(0.7)/Ni@CNTs)was synthesized by a facile one-step pyrolysis protocol.Experimental and theoretical results demonstrated that the electronic coupling interaction between Ni and Ni_(3)ZnC_(0.7) triggered the redistribution of interfacial charge and optimized the electronic state density of metallic Ni sites,which reduced the H^(*) adsorption–desorption energy barrier and thus accelerated the HER kinetics in the electrocatalytic process.The resulting Ni_(3)ZnC_(0.7)/Ni@CNTs required ultralow overpotentials of 93 and 256 mV to deliver current densities of 10 and 100 mA cm^(−2) for the HER,respectively,and exhibited extraordinary long-term durability for at least 400 h in 1.0 M KOH solution.This work provides a novel perspective for the design of high-performance bimetallic carbide electrocatalysts for water splitting.
