Currently most of research efforts for selective electrocatalysis CO_(2) reduction to C2+products have relied on crystalline Cu-based catalysts;amorphous Cu with abundant low-coordinated atoms holds greater promise fo...Currently most of research efforts for selective electrocatalysis CO_(2) reduction to C2+products have relied on crystalline Cu-based catalysts;amorphous Cu with abundant low-coordinated atoms holds greater promise for this conversion yet remains relatively underexplored.Here we report an amorphous urchin-like Cu@nanosilica hybrid synthesized by electrostatic coupling Si polyanions with Cu salt in hydrothermal processes.The Cu@nanosilica electrocatalyst displays excellent CO_(2) electroreduction activity and selectivity with a Faradic efficiency of 70.5%for C2+product production,and higher stability compared to the crystalline Cu counterpart.The solar-driven CO_(2) electrolysis yields an energy efficiency of 20%for C2+product production.Mechanism study reveals that the urchin-like Cu@nanosilica catalyst with amorphous Cu/Cu^(+)dispersion enhances CO_(2) adsorption and activation to facilitate generation of CO_(2)^(-)*and possible CO^(*)intermediates,and suppresses hydrogen evolution concurrently.The combined effects of both aspects promote efficient C2+product production from CO_(2) electroreduction.展开更多
基金supported by the National Natural Science Foundation of China(No.21872147 and 21805277)the Natural Science Foundation of Fujian Province(No.2018J05030 and 2019J05152)+2 种基金the Key Research Program of Frontier Sciences,CAS(No.ZDBSLY-SLH028)the DNL Cooperation Fund,CAS(DNL201924)the Strategic Priority Research Program,CAS(No.XDB20000000)。
文摘Currently most of research efforts for selective electrocatalysis CO_(2) reduction to C2+products have relied on crystalline Cu-based catalysts;amorphous Cu with abundant low-coordinated atoms holds greater promise for this conversion yet remains relatively underexplored.Here we report an amorphous urchin-like Cu@nanosilica hybrid synthesized by electrostatic coupling Si polyanions with Cu salt in hydrothermal processes.The Cu@nanosilica electrocatalyst displays excellent CO_(2) electroreduction activity and selectivity with a Faradic efficiency of 70.5%for C2+product production,and higher stability compared to the crystalline Cu counterpart.The solar-driven CO_(2) electrolysis yields an energy efficiency of 20%for C2+product production.Mechanism study reveals that the urchin-like Cu@nanosilica catalyst with amorphous Cu/Cu^(+)dispersion enhances CO_(2) adsorption and activation to facilitate generation of CO_(2)^(-)*and possible CO^(*)intermediates,and suppresses hydrogen evolution concurrently.The combined effects of both aspects promote efficient C2+product production from CO_(2) electroreduction.
