CoCu双原子驱动的高效电催化甲烷制甲醇

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中图分类号：0643 文献标志码：A

Abstract：Thefirst-principlesdensityfunctionaltheorycalculationswasusedtoivestigatetheperformanceofdual-atomcatalysts（DACs）anchored on a Mo2CO2 MXene substrate（denoted as M1M2/Mo2CO2 ，where M1=Fe，Co，Ni and M2=Co ， ΔNi，Cu） for the electrocatalytic conversion of methane （ CH4 ）tomethanol（ CH3OH ）.The stability of the catalysts was assessedviaformationenergyanddisolutionpotentialcalculations.Thecatalyticactivityandselectivitywereprobedthrough reactionfreeenergyanalysis.Theoriginofcatalyticactivitywas elucidatedviaelectronicstructureanalysis.Itisfoundthat the formation energy of M1M2/Mo2CO2 catalyst is from -4.44eV to -2.62eV ，and the dissolution potential is between 1.03 V and 1.77V ，exhibiting excellent thermodynamicand electrochemical stability.Among them，the activation energy barrier of methane on CoCu/Mo2CO2 is only 0.05eV ，indicating excellent catalytic activity.Within a potential windowof 0.74V to 1.01V （vs.RHE），this catalyst achieves methanol selectivity exceeding 99% .Thecatalytic activity shows a positive correlation with the charge ratio （q（M1）/q（M2））， ）of the dual-metal centers.The high activity of CoCu/Mo2CO2 originates from its q（M1）/q（M2） ratio of O.3，which is close to the theoretical optimumvalue.

Keywords：first principles；methane to methanol；diatomic catalysts；electrocatalysis

甲烷作为重要的化学原料之一，是许多化学品生产的基础，且可以通过天然气、页岩气等方便获得[1-3]。（剩余13951字）