Abstract
The engineering of the electronic configurations of active sites,together with the production of more accessible active sites through heterostructure design,has been established as a forceful methodology for boosting water electrolysis performance.Herein,a facile approach is developed to fabricate well-dispersed MoO2 and WO2 nanoparticles with abundant heterointerfaces entrapped in N,P-doped carbon nanofibers(referred to as MoO2/WO2@N,P-CNFs hereafter)as hydrogen evolution reaction(HER)electrocatalysts in alkaline and acidic electrolytes.Extensive spectroscopic analyses and theoretical findings manifest that the heterointerface formed by the work function modulation of MoO2/WO2 triggers the sponta-neous electron redistribution from MoO2 to WO2 and a built-in electric field,which is essential to promote water adsorption,optimize the H-intermediate adsorption energy,result in the enhanced charge transfer efficiency,and ulti-mately increase the intrinsic HER activity.Simultaneously,the intimate confinement of MoO2/WO2 heterostructures in the porous carbon substrate can restrain the active sites from unfavorable coarsening and detachment,thus ensur-ing facilitated HER kinetics and outstanding structural robustness.As a result,MoO2/WO2@N,P-CNFs exhibit superior catalytic HER performance in acidic and basic solutions,requiring 118 and 95 mV overpotentials to achieve 10 mA·cm-2,respectively,surpassing a number of reported non-noble metal-based electrocatalysts.This work provides guidelines for the rational design and construction of special metallic heterocomponents with optimized interfacial electronic structure for various electrochemical technologies.
基金项目
国家自然科学基金(U21A20332)
国家自然科学基金(52103226)
国家自然科学基金(52202275)
国家自然科学基金(52203314)
国家自然科学基金(12204253)
Distinguished Young Scholars Fund of Jiangsu Province(BK20220061)