The AgOCH3- and Ag-（CH3OH）x（x=l, 2） anions are studied by photoelectron imaging as well as ab initio calculations. The adiabatic and vertical detachment energies （ADE and VDE） of AgOCH3- are determined as 1.29（...The AgOCH3- and Ag-（CH3OH）x（x=l, 2） anions are studied by photoelectron imaging as well as ab initio calculations. The adiabatic and vertical detachment energies （ADE and VDE） of AgOCH3- are determined as 1.29（2） and 1.34（2） eV, respectively, from the vibrational resolved photoelectron spectrum. The Ag-（CH3OH）l,2 anionic complexes are characterized as metal atomic anion solvated by the CH3OH molecules with the electron mainly localized on the metal. The photoelectron spectra of Ag-（CH3OH）x （x=O, 1, 2） show a gradual increase in VDE with increasing x, due to the solvent stabilization. Evidence for the methanol-methanol hydrogen bonding interactions appears when the Ag- is solvated by two methanol molecules.展开更多
Inspired by the recent experimental synthesis of graphene nanoribbons （GNKs） and theoretical research on their edge-decoration, we comprehensively studied the electrocatalytic performance of GNRs edge-decorated with...Inspired by the recent experimental synthesis of graphene nanoribbons （GNKs） and theoretical research on their edge-decoration, we comprehensively studied the electrocatalytic performance of GNRs edge-decorated with Cu for CO2 reduction. Compared to zigzag GNRs, the Cu-terminated armchair GNRs with a width of n = 3p ＋ 2 were more efficient catalysts for producing methanol from CO2 with a free energy barrier of less than 0.5 eV, offering the advantages of a lower overpotential and higher selectivity than bulk Cu and other graphene-supported Cu structures. On the other hand, the competing hydrogen evolution reaction could be effectively suppressed by Cu-terminated armchair GNRs. Hence, the edge-decorated GNRs offer great flexibility for tuning the catalytic efficiency and selectivity for CO2 electroreduction.展开更多
基金This work was supported by the National Natural Science Foundation of China （No.20933003 and No.21073186） and the National Basic Research Program of China （No.2007CBSI5203, No.2010CB732306, and No.2007CBSI5201）.
文摘The AgOCH3- and Ag-（CH3OH）x（x=l, 2） anions are studied by photoelectron imaging as well as ab initio calculations. The adiabatic and vertical detachment energies （ADE and VDE） of AgOCH3- are determined as 1.29（2） and 1.34（2） eV, respectively, from the vibrational resolved photoelectron spectrum. The Ag-（CH3OH）l,2 anionic complexes are characterized as metal atomic anion solvated by the CH3OH molecules with the electron mainly localized on the metal. The photoelectron spectra of Ag-（CH3OH）x （x=O, 1, 2） show a gradual increase in VDE with increasing x, due to the solvent stabilization. Evidence for the methanol-methanol hydrogen bonding interactions appears when the Ag- is solvated by two methanol molecules.
文摘Inspired by the recent experimental synthesis of graphene nanoribbons （GNKs） and theoretical research on their edge-decoration, we comprehensively studied the electrocatalytic performance of GNRs edge-decorated with Cu for CO2 reduction. Compared to zigzag GNRs, the Cu-terminated armchair GNRs with a width of n = 3p ＋ 2 were more efficient catalysts for producing methanol from CO2 with a free energy barrier of less than 0.5 eV, offering the advantages of a lower overpotential and higher selectivity than bulk Cu and other graphene-supported Cu structures. On the other hand, the competing hydrogen evolution reaction could be effectively suppressed by Cu-terminated armchair GNRs. Hence, the edge-decorated GNRs offer great flexibility for tuning the catalytic efficiency and selectivity for CO2 electroreduction.
