Conversion of Catalytically Inert 2D Bismuth Oxide Nanosheets for Effective Electrochemical Hydrogen Evolution Reaction Catalysis via Oxygen Vacancy Concentration Modulation

作     者：Ziyang Wu Ting Liao Sen Wang Janith Adikaram Mudiyanselage Aaron SMicallef Wei Li Anthony PO’Mullane Jianping Yang Wei Luo Kostya Ostrikov Yuantong Gu Ziqi Sun Ziyang Wu;Ting Liao;Sen Wang;Janith Adikaram Mudiyanselage;Aaron S.Micallef;Wei Li;Anthony P.O'Mullane;Jianping Yang;Wei Luo;Kostya Ostrikov;Yuantong Gu;Ziqi Sun

作者机构：School of MechanicalMedical and Process EngineeringQueensland University of Technology2 George StreetBrisbaneQLD 4000Australia Centre for Materials ScienceQueensland University of Technology2 George StreetBrisbaneQLD 4000Australia School of Earth and Atmospheric SciencesQueensland University of Technology2 George StreetBrisbaneQLD 4000Australia School of Chemistry and PhysicsQueensland University of Technology2 George StreetBrisbaneQLD 4000Australia Central Analytical Research FacilityQueensland University of Technology2 George StreetBrisbaneQLD 4000Australia State Key Laboratory for Modification of Chemical Fibers and Polymer MaterialsCollege of Materials Science and EngineeringDonghua UniversityShanghai 201620People’s Republic of China 

出 版 物：《Nano-Micro Letters》 (纳微快报（英文版）)

年 卷 期：2022年第14卷第6期

页      面：48-64页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：This work was financially supported by the Australian Research Council(ARC)through Future Fellowship grants(FT180100387 and FT160100281) Discovery Projects(DP200103568,DP210100472,and DP200102546) WL thanks the support of the Science and Technology Commission of Shanghai Municipality(19520713200) Open access funding provided by Shanghai Jiao Tong University 

主　　题：Alkaline hydrogen evolution reaction Bismuth oxide Plasma irradiation 2D materials Oxygen vacancy 

摘      要：Oxygen vacancies(Vo)in electrocatalysts are closely correlated with the hydrogen evo-lution reaction(HER)*** role of vacancy defects and the effect of their concentration,how-ever,yet remains ***,Bi2O3,an unfavorable electrocata-lyst for the HER due to a less than ideal hydrogen adsorption Gibbs free energy(ΔGH*),is utilized as a perfect model to explore the func-tion of Vo on HER *** a facile plasma irradia-tion strategy,Bi2O3 nanosheets with different Vo concentrations are fabricated to evaluate the influence of defects on the HER ***,while the generated oxygen vacancies contribute to the enhanced HER performance,higher Vo concentrations beyond a saturation value result in a significant drop in HER *** tunning the Vo concentration in the Bi_(2)O_(3)nanosheets via adjusting the treatment time,the Bi2O3 catalyst with an optimized oxygen vacancy concentration and detectable charge carrier concentration of 1.52×10^(24)cm^(−3)demonstrates enhanced HER performance with an overpotential of 174.2 mV to reach 10 mA cm^(−2),a Tafel slope of 80 mV dec−1,and an exchange current density of 316 mA cm−2 in an alkaline solution,which approaches the top-tier activity among Bi-based HER ***-functional theory calculations confirm the preferred adsorption of H*onto Bi2O3 as a function of oxygen chemical potential(ΔμO)and oxygen partial potential(PO2)and reveal that high Vo concentrations result in excessive stability of adsorbed hydrogen and hence the inferior HER *** study reveals the oxygen vacancy concentration-HER catalytic activity relationship and provides insights into activating catalytically inert materials into highly efficient electrocatalysts.