单分散Cu-TCPP/Cu2O杂化微球:一种具有优异电还原CO2产C2性能的级联电催化剂OA北大核心CSTPCD

The electrochemical conversion of carbon dioxide(CO2)into valuable chemicals is a feasible way to mitigate the negative impacts of overmuch CO2 emissions.Porphyrin-based metal organic frameworks(MOFs)are expected to be used for selective and efficient electrochemical CO2 reduction(ECR)with porous structure and ordered active sites.Herein,we report the synthesis of a monodispersed and spherical organic/inorganic hybrid Cu-TCPP@Cu2O elec-trocatalyst composed of Cu-TCPP(TCPP=tetrakis(4-carboxyphenyl)porphyrin)and Cu2O,where TCPP plays significant roles in regulating the morphology.In-situ formed Cu during ECR process in combination with Cu-TCPP(Cu-TCPP@Cu)can suppress hydrogen evolution,enrich CO intermediate and promote C-C coupling toward C2 products.The Cu-TCPP@Cu supported on porous carbon(PC)showed ultrafine Cu nanoclusters on PC,and dis-played high ECR activity and selectivity toward C2 products,with a C2 faradaic efficiency of 62.3％at-1.0 V versus the reversible hydrogen electrode and a C2 partial current density of 83.4 mA.cm-2,which is 7.6 times and 13.1 times those of pure Cu2O and TCPP,respectively.The morphology and hybrid structure of the catalyst were studied to improve the selectivity of ECR to produce C2 products,which provides a new idea for the design of high-performance ECR catalyst.