Metal-organic frameworks(MOFs)are a unique class of crystalline porous materials composed of metal nodes and organic linkers(Figure 1a),featuring tunable pore structures,high surface areas,and well-defined coordinatio...Metal-organic frameworks(MOFs)are a unique class of crystalline porous materials composed of metal nodes and organic linkers(Figure 1a),featuring tunable pore structures,high surface areas,and well-defined coordination environments[1].These attributes make MOFs an emerging family of electrocatalysts,offering atomiclevel control over active sites and structural modularity that is difficult to achieve with conventional catalysts[2].In particular,MOFs have shown promise as oxygen evolution reaction(OER)electrocatalysts for alkaline water electrolysis owing to their ability to host abundant and low-cost transition-metal elements such as Co,Ni,and Fe[3].展开更多
t is important but still challenging to reveal the effect of precise structural modification of polyoxometalates(POMs)on electrocatalytic hydrogen evolution reaction(HER).Here,we present the syntheses of five polyoxon...t is important but still challenging to reveal the effect of precise structural modification of polyoxometalates(POMs)on electrocatalytic hydrogen evolution reaction(HER).Here,we present the syntheses of five polyoxoniobate(PONb)analogs with well-defined structures,including Na-GeNb_(12),Cu-GeNb_(12),GeV_(2)Nb_(12),V_(3)Nb_(12),and SiV_(2)Nb_(12),as model systems,enabling us to unravel the effects of structural modification of POMs on the electrocatalytic HER at the atomic level.Our results revealed that the bridging O atoms of PONbs were the primary active sites for HER,whose catalytic performance was mostly affected by the central atom of PONb,followed by surface composition and then by counterion.Comprehensive characterizations and theoretical calculations were performed to confirm and interpret the above findings,which provide a rational atomic-level design of efficient POM-based HER electrocatalysts.展开更多
文摘Metal-organic frameworks(MOFs)are a unique class of crystalline porous materials composed of metal nodes and organic linkers(Figure 1a),featuring tunable pore structures,high surface areas,and well-defined coordination environments[1].These attributes make MOFs an emerging family of electrocatalysts,offering atomiclevel control over active sites and structural modularity that is difficult to achieve with conventional catalysts[2].In particular,MOFs have shown promise as oxygen evolution reaction(OER)electrocatalysts for alkaline water electrolysis owing to their ability to host abundant and low-cost transition-metal elements such as Co,Ni,and Fe[3].
基金supported by the financial support from the National Natural Science Foundation of China(NSFC,grant nos.22109164,21971039,and 21973013)the Key Program of Natural Science Foundation of Fujian Province,China(grant no.2021J02007).
文摘t is important but still challenging to reveal the effect of precise structural modification of polyoxometalates(POMs)on electrocatalytic hydrogen evolution reaction(HER).Here,we present the syntheses of five polyoxoniobate(PONb)analogs with well-defined structures,including Na-GeNb_(12),Cu-GeNb_(12),GeV_(2)Nb_(12),V_(3)Nb_(12),and SiV_(2)Nb_(12),as model systems,enabling us to unravel the effects of structural modification of POMs on the electrocatalytic HER at the atomic level.Our results revealed that the bridging O atoms of PONbs were the primary active sites for HER,whose catalytic performance was mostly affected by the central atom of PONb,followed by surface composition and then by counterion.Comprehensive characterizations and theoretical calculations were performed to confirm and interpret the above findings,which provide a rational atomic-level design of efficient POM-based HER electrocatalysts.
