摘要
Simultaneously achieving high activity,selectivity and stability for electrochemical CO_(2)reduction reaction(CO_(2)RR)remains great challenges.Herein,a phosphorus-modified Sn/Sn Oxcore/shell(P-Sn/SnO_x)catalyst,derived from in situ electrochemical reduction of an amorphous Sn(HPO_(4))_(2) pre-catalyst,exhibits high CO_(2)RR performance.The total Faradaic efficiency(FE)of C_(1) products is close to 100%in a broad potential range from-0.49 to-1.02 V vs.reversible hydrogen electrode,and a total current density of 315.0 m A cm^(-2)is achieved.Moreover,the P-Sn/SnO_(x) catalyst maintains a formate FE of~90%for 120 h.Density functional theory calculations suggest that the phosphorus-modified Sn/SnO_(x) core/shell structure effectively facilitates formate production by enhancing CO_(2)adsorption and improving free energy profile of formate formation.
基金
supported by the National Key R&D Program of China (2021YFA1501503)
the National Natural Science Foundation of China (22125205,22002155,22002158,92045302)
the“Transformational Technologies for Clean Energy and Demonstration”Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21070613)
the Fundamental Research Funds for the Central Universities (20720220008)
the China Postdoctoral Science Foundation (2019M661142)
the Natural Science Foundation of Liaoning Province (2021-MS-022)
the High-Level Talents Innovation Project of Dalian City (2020RQ038)
the support from the Photon Science Center for Carbon Neutrality。
