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 

机构地区：[1]Guangxi Key Laboratory of Low Carbon Energy Materials,School of Chemistry and Pharmaceutical Sciences,Guangxi Normal University,Guilin 541004,Guangxi,China [2]Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST),Thuwal 23955-6900,Saudi Arabia

出　　处：《Journal of Energy Chemistry》2022年第9期395-404,I0011,共11页能源化学（英文版）

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)。

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.

关 键 词：Ru/Ni-NiO@C Vacancy defects Electrocatalysis Metal-organic framework Hydrogen oxidation 

分 类 号：O643.36[理学—物理化学] TM911.4[理学—化学]