摘要
Molecular catalysts can effectively steer the electrocatalytic acetylene semihydrogenation into ethylene,but realizing high Faradaic efficiency(FE)at industrial current densities remains a challenge.Herein,we report a ligand engineering strategy that utilizes polymeric N–heterocyclic carbene(NHC)as a hydrophobic ligand to modulate the microenvironment of Cu sites.This polymeric NHC imparts appropriate hydrophobic properties for the chelated Cu sites,thereby moderating the H_(2)O transport and enabling easy access of acetylene.Consequently,the polymeric NHC chelated Cu exhibits an FE_(ethylene)of~97%at a current density of 500 m A/cm^(2)in a flow cell.Particularly in a zero-gap reactor,the FE_(ethylene)consistently exceeds 86%across current densities from 100 m A/cm^(2)to 400 m A/cm^(2),reaching an optimal FEethyleneof 98%at 200 m A/cm^(2)and achieving durable operation for 155 h at 100 m A/cm^(2).This work provides a promising paradigm to regulate the microenvironment of molecular catalysts for improving electrocatalytic performances under industrial current densities.
基金
supported by the National Natural Science Foundation of China(Nos.22475170,52101271,22375166)
the Guangdong Basic and Applied Basic Research Foundation(Nos.2020A1515111017,2024A1515011977)
the Key Research and Development Program of Shaanxi Province(No.2024GX-YBXM379)。
