Delicate surface vacancies engineering of Ru doped MOF-derived Ni-NiO@C hollow microsphere superstructure to achieve outstanding hydrogen oxidation performance

作     者：Yuting Yang Yi Huang Shuqing Zhou Yi Liu Luyan Shi Tayirjan Taylor Isimjan Xiulin Yang Yuting Yang;Yi Huang;Shuqing Zhou;Yi Liu;Luyan Shi;Tayirjan Taylor Isimjan;Xiulin Yang

作者机构：Guangxi Key Laboratory of Low Carbon Energy MaterialsSchool of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Saudi Arabia 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2022年第31卷第9期

页      面：395-404,I0011页

核心收录：

学科分类：0808[工学-电气工程] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 0806[工学-冶金工程] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 0702[理学-物理学] 

基　　金：supported by the National Natural Science Foundation of China(21965005) the Natural Science Foundation of Guangxi Province(2018GXNSFAA294077,2021GXNSFAA076001) the Project of High-Level Talents of Guangxi(F-KA18015) the Guangxi Technology Base and Talent Subject(GUIKEAD18126001,GUIKE AD20297039)。 

主　　题：Ru/Ni-NiO@C Vacancy defects Electrocatalysis Metal-organic framework Hydrogen oxidation 

摘      要：Surface vacancy defects,as the bridge between theoretical structural study and the design of heterogenous catalysts,have captured much attention.This work develops a metal-organic framework-engaged replacement-pyrolysis approach to obtain highly dispersed Ru nanoparticles immobilized on the vacancy-rich Ni-NiO@C hollow microsphere(Ru/Ni-NiO@C).Fine annealing at 400°C introduces nickel and oxygen vacancies on Ru/Ni-NiO@C surface,resulting in an improved electrical conductivity and rapid mass-charge transfer efficiency.Ru/Ni-NiO@C with a hollow micro/nanostructure and interconnected meso-porosity favors the maximal exposure of abundant active sites and elevation of hydrogen oxidation reaction(HOR)activity.Experimental results and density functional theory(DFT)calculations reveal that an electronic effect between Ru and Ni-NiO@C,in conjunction with nickel/oxygen vacancies in the NiO species could synergistically optimize hydrogen binding energy(HBE)and hydroxide binding energy(OHBE).The HBE and OHBE optimizations thus created confer Ru/Ni-NiO@C with a mass activity over 7.75 times higher than commercial Pt/C.Our work may provide a constructive route to make a breakthrough in elevating the hydrogen electrocatalytic performance.