Electrochemical semihydrogenation of acetylene(C_(2)H_(2))using renewable electricity offers a sustainable route for ethylene(C_(2)H_(4))production.However,the development of this technique has been hindered by many c...Electrochemical semihydrogenation of acetylene(C_(2)H_(2))using renewable electricity offers a sustainable route for ethylene(C_(2)H_(4))production.However,the development of this technique has been hindered by many challenges,such as competitive hydrogen evolution reactions(HERs)and overhydrogenation at high current densities,which will reduce the faradaic efficiency(FE)of C_(2)H_(4) and negatively impact downstream processing.Herein,we develop defectrich copper nanocubes(v-Cu NCs)as efficient electrocatalysts that facilitateC_(2)H_(4) adsorption while suppressing HER and overhydrogenation.The superior semihydrogenation performances are verified by the high C_(2)H_(4) FE of 98.3%at an ultrahigh current density of 0.7 A cm^(−2).Remarkably,in a 25 cm^(2) electrolyzer,v-Cu NCs deliver a record-high single-pass conversion of 97.5%forC_(2)H_(4) and C_(2)H_(4) selectivity of 97.4%at a cathode current of 1.6 A with a flow rate of 10 mL min−1,operating stably for 50 h.In-situ Raman spectroscopy and theoretical calculations reveal that uniformly oriented Cu(100)planes and nitrogen vacancies generate strongC_(2)H_(4) adsorption at copper sites,which facilitates hydrogenation kinetics and increases the energy barrier for overhydrogenation.This work offers valuable insights into the implementation ofC_(2)H_(4)-to-C_(2)H_(4) production and the development of efficient electrocatalysts forC_(2)H_(4) semihydrogenation.展开更多
基金supported by the National Natural Science Foundation of China(grant nos.22322807,22168023,22268029,and 22108243)the Natural Science Foundation of Jiangxi Province(grant no.20224ACB204003)+1 种基金the China Scholarship Council(grant no.202206820025)the Australian Research Council(ARC)through the ARC Discovery project(grant no.DP230101579).
文摘Electrochemical semihydrogenation of acetylene(C_(2)H_(2))using renewable electricity offers a sustainable route for ethylene(C_(2)H_(4))production.However,the development of this technique has been hindered by many challenges,such as competitive hydrogen evolution reactions(HERs)and overhydrogenation at high current densities,which will reduce the faradaic efficiency(FE)of C_(2)H_(4) and negatively impact downstream processing.Herein,we develop defectrich copper nanocubes(v-Cu NCs)as efficient electrocatalysts that facilitateC_(2)H_(4) adsorption while suppressing HER and overhydrogenation.The superior semihydrogenation performances are verified by the high C_(2)H_(4) FE of 98.3%at an ultrahigh current density of 0.7 A cm^(−2).Remarkably,in a 25 cm^(2) electrolyzer,v-Cu NCs deliver a record-high single-pass conversion of 97.5%forC_(2)H_(4) and C_(2)H_(4) selectivity of 97.4%at a cathode current of 1.6 A with a flow rate of 10 mL min−1,operating stably for 50 h.In-situ Raman spectroscopy and theoretical calculations reveal that uniformly oriented Cu(100)planes and nitrogen vacancies generate strongC_(2)H_(4) adsorption at copper sites,which facilitates hydrogenation kinetics and increases the energy barrier for overhydrogenation.This work offers valuable insights into the implementation ofC_(2)H_(4)-to-C_(2)H_(4) production and the development of efficient electrocatalysts forC_(2)H_(4) semihydrogenation.
