The hydrogen evolution reaction(HER) through electrocatalysis is promising for the production of clean hydrogen fuel. However,designing the structure of catalysts,controlling their electronic properties,and manipulati...The hydrogen evolution reaction(HER) through electrocatalysis is promising for the production of clean hydrogen fuel. However,designing the structure of catalysts,controlling their electronic properties,and manipulating their catalytic sites are a significant challenge in this field. Here,we propose an electrochemical surface restructuring strategy to design synergistically interactive phosphorus-doped carbon@MoP electrocatalysts for the HER. A simple electrochemical cycling method is developed to tune the thickness of the carbon layers that cover on MoP core,which significantly influences HER performance. Experimental investigations and theoretical calculations indicate that the inactive surface carbon layers can be removed through electrochemical cycling,leading to a close bond between the MoP and a few layers of coated graphene. The electronsdonated by the MoP core enhance the adhesion and electronegativity of the carbon layers;the negatively charged carbon layers act as an active surface. The electrochemically induced optimization of the surface/interface electronic structures in the electrocatalysts significantly promotes the HER. Using this strategy endows the catalyst with excellent activity in terms of the HER in both acidic and alkaline environments(current density of 10 mA cm^(-2) at low overpotentials,of 68 mV in 0.5 M H_(2)SO_(4) and 67 mV in 1.0 M KOH).展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos. 21975286 and 21473254)the Special Project Fund of “Taishan Scholar” of Shandong Province (Grant No. ts201511017)+2 种基金the QLUT Special Funding for Distinguished Scholars (Grant No. 2419010420)the project ZR2020QE058 supported by Shandong Provincial Natural Science Foundationthe Fundamental Research Funds for the Central Universities (Grant Nos. YCX2020050,18CX06030A,and 17CX02039A)。
文摘The hydrogen evolution reaction(HER) through electrocatalysis is promising for the production of clean hydrogen fuel. However,designing the structure of catalysts,controlling their electronic properties,and manipulating their catalytic sites are a significant challenge in this field. Here,we propose an electrochemical surface restructuring strategy to design synergistically interactive phosphorus-doped carbon@MoP electrocatalysts for the HER. A simple electrochemical cycling method is developed to tune the thickness of the carbon layers that cover on MoP core,which significantly influences HER performance. Experimental investigations and theoretical calculations indicate that the inactive surface carbon layers can be removed through electrochemical cycling,leading to a close bond between the MoP and a few layers of coated graphene. The electronsdonated by the MoP core enhance the adhesion and electronegativity of the carbon layers;the negatively charged carbon layers act as an active surface. The electrochemically induced optimization of the surface/interface electronic structures in the electrocatalysts significantly promotes the HER. Using this strategy endows the catalyst with excellent activity in terms of the HER in both acidic and alkaline environments(current density of 10 mA cm^(-2) at low overpotentials,of 68 mV in 0.5 M H_(2)SO_(4) and 67 mV in 1.0 M KOH).
