Interfacial Ru nanoclusters in tandem with single atoms on oxygen-vacancy regulated CeO_(2)for anion exchange membrane seawater-splitting  

作　　者：Yue Wang Jing Li Pengfei Yang Hongdong Li Guangrui Xu Yunmei Du Caixia Li Wei Jin Tianyi Ma Zexing Wu Lei Wang 

机构地区：[1]Key Laboratory of Eco-chemical Engineering,Ministry of Education,International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing,College of Chemistry and Molecular Engineering,College of Chemical Engineering,Qingdao University of Science&Technology,Qingdao 266042,Shandong,China [2]College of Chemical Engineering,Qingdao University of Science and Technology,Qingdao 266042,Shandong,China [3]College of Materials Science and Engineering,Qingdao University of Science&Technology,Qingdao 266042,Shandong,China [4]College of Environment and Safety Engineering,Qingdao University of Science and Technology,Qingdao 266042,Shandong,China [5]School of Environmental Science and Engineering,Suzhou University of Science and Technology,Suzhou 215009,Jiangsu,China [6]School of Science,STEM College,RMIT University 3083,Victoria,Australia

出　　处：《Journal of Energy Chemistry》2025年第3期618-627,共10页能源化学(英文版)

基　　金：funding support from the National Natural Science Foundation of China(52371227;22002068;52272222,and 52072197);the Taishan Scholar Young Talent Program(tsqn201909114);the Shandong Province“Double-Hundred Talent Plan”(WST2020003);the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(2019KJC004);the Outstanding Youth Foundation of Shandong Province,China(ZR2019JQ14);the Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant No.ZR2020ZD09;the Major Scientific and Technological Innovation Project(2019JZZY020405);the University Youth Innovation Team of Shandong Province(202201010318);the Youth Innovation Team Development Program of Shandong Higher Education Institutions(2022KJ155)。

摘　　要：A hydrogen spillover-bridged water dissociation/hydrogen formation could concurrently promote Volmer/Tafel process and improve the efficiency of hydrogen evolution reaction(HER)under alkaline conditions.However,it is still challenging to promote occurrence of hydrogen spillover for the large interfacial transport barriers of H_(2)O and hydrogen on active sites.Herein,the strategy of energy barrier gradient to induce hydrogen spillover was proposed by constructing Ru nanoclusters coupled with single atom onto oxygen vacancy cerium dioxide(Ru/CeO_(2)-Ov-2).Density functional theory(DFT)calculations uncover that the adsorption/desorption of H2O occurs at the Ru clusters sites and then the dissociated H*spontaneously overflows from Ru clusters with high binding energy into the adjacent Ru single atom sites with low binding energy,which facilitate the hydrogen formation.Consequently,the synthesized Ru/CeO_(2)-Ov-2 exhibits a small overpotential of 41 mV at 10 mA cm^(-2)and good stability at 500 mA cm^(-2)for 100 h in alkaline seawater,which could be ascribed to the rapid hydrogen spillover and strong coupling interaction between Ru and CeO_(2)-O_(v).This work provides a novel insight that synthesizing cooperative sites with energy barrier gradient helps to promote hydrogen spillover and accelerate the Volmer/Tafel process of HER.

关 键 词：ELECTROCATALYST CeO_(2) RU Oxygen vacancy Hydrogen evolution reaction 

分 类 号：O643.36[理学—物理化学]