Performance breakthrough of electrocatalysts highly relies on the regulation of internal structures and electronic states.In present work,for the first time,we successfully synthesized nitrogen doped FeS_(2) nanoparti...Performance breakthrough of electrocatalysts highly relies on the regulation of internal structures and electronic states.In present work,for the first time,we successfully synthesized nitrogen doped FeS_(2) nanoparticles(N-FeS_(2))as the electrocatalysts for hydrogen evolution reaction(HER).The band structure and electronic state of FeS_(2) are modulated by a nitrogen doping strategy,as confirmed by X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS)and density functional theory(DFT)calculations.Owing to the band structure and electronic state regulation as well as the weakening of H-S interaction,the designed N-FeS_(2) electrocatalyst exhibits superior catalytic performance with a low overpotential(~126 mV at 10 mA cm^(-2))and excellent activity stability under alkaline conditions,which is substantially improved as compared with that of the pure FeS_(2) counterpart.Our work demonstrates that the modulation of electron state and band structure of an electrocatalyst,which can provide a valuable guidance for designing excellent catalysts for hydrogen evolution reaction and beyond.展开更多
基金supported by National Key R&D Program of China(2017YFA0403402,2017YFA0700104)the National Natural Science Foundation of China(Grant Nos.11875258 and U1732232)+2 种基金the DNL Cooperation Fund,CAS(DNL180201)the Fundamental Research Funds for the Central Universities(Nos.WK2060190081)Users with Excellence Program of Hefei Science Center CAS(Nos.2018HSC-UE003 and 2019HSC-UE004)。
文摘Performance breakthrough of electrocatalysts highly relies on the regulation of internal structures and electronic states.In present work,for the first time,we successfully synthesized nitrogen doped FeS_(2) nanoparticles(N-FeS_(2))as the electrocatalysts for hydrogen evolution reaction(HER).The band structure and electronic state of FeS_(2) are modulated by a nitrogen doping strategy,as confirmed by X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS)and density functional theory(DFT)calculations.Owing to the band structure and electronic state regulation as well as the weakening of H-S interaction,the designed N-FeS_(2) electrocatalyst exhibits superior catalytic performance with a low overpotential(~126 mV at 10 mA cm^(-2))and excellent activity stability under alkaline conditions,which is substantially improved as compared with that of the pure FeS_(2) counterpart.Our work demonstrates that the modulation of electron state and band structure of an electrocatalyst,which can provide a valuable guidance for designing excellent catalysts for hydrogen evolution reaction and beyond.