Solar-driven CO_(2)conversion to multicarbon(C_(2+))products has emerged as a key challenge,yet this calls for a systematic investigation on the overall reaction process and mechanism at an atomic level based on the r...Solar-driven CO_(2)conversion to multicarbon(C_(2+))products has emerged as a key challenge,yet this calls for a systematic investigation on the overall reaction process and mechanism at an atomic level based on the rational design of highly selective photocatalysts.Herein,we report the synthesis of compact Bi_(2)S_(3)/Cds heterostructures via facile cation exchange,by which a unique pathway of CO_(2)-to-C_(2)H_(4) photoconversion is achieved.Specifically,the BCS-30 shows an optimal C_(2)H_(4) production rate of 3.49μmolh^(-1)g^(-1) based on the regulation of band structures and energy levels of photocatalysts by controlled growth of Bi_(2)S_(3) at CdS surface.Both experimental and theoretical results(DFT calculations)identify Bi atoms as new catalytic sites for the adsorption of CO*and formation of*CO-*CO dimers that further hydrogenate to produce ethylene.Overall,this work demonstrates vast potentials of delicately designed heterostructures for CO_(2) conversion towards C_(2+)products under mild photocatalytic conditions.展开更多
基金supported by the NSFC(nos.91622114,21520102001,21521061,and 21331006)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(grant no.SKLPEE-202008)Fuzhou University,and the Special Fund for Scientific and Technological Innovation of Fujian Agriculture and Forestry University(grant no.CXZX2019073G).
文摘Solar-driven CO_(2)conversion to multicarbon(C_(2+))products has emerged as a key challenge,yet this calls for a systematic investigation on the overall reaction process and mechanism at an atomic level based on the rational design of highly selective photocatalysts.Herein,we report the synthesis of compact Bi_(2)S_(3)/Cds heterostructures via facile cation exchange,by which a unique pathway of CO_(2)-to-C_(2)H_(4) photoconversion is achieved.Specifically,the BCS-30 shows an optimal C_(2)H_(4) production rate of 3.49μmolh^(-1)g^(-1) based on the regulation of band structures and energy levels of photocatalysts by controlled growth of Bi_(2)S_(3) at CdS surface.Both experimental and theoretical results(DFT calculations)identify Bi atoms as new catalytic sites for the adsorption of CO*and formation of*CO-*CO dimers that further hydrogenate to produce ethylene.Overall,this work demonstrates vast potentials of delicately designed heterostructures for CO_(2) conversion towards C_(2+)products under mild photocatalytic conditions.
