Solar-driven CO_(2)conversion to prepare value-added products is highly desirable but challenging.Central to the achievement of multi-carbon products via CO_(2)photoconversion is to break the bottlenecks of C-C coupli...Solar-driven CO_(2)conversion to prepare value-added products is highly desirable but challenging.Central to the achievement of multi-carbon products via CO_(2)photoconversion is to break the bottlenecks of C-C coupling and multi-electron transfer.Herein,a charge relay system consisting of Pd-decorated BiOCl-wrapped CuBi_(2)O_(4)is reported by taking advantage of the synergy of Pd nanoparticles(PdNPs)and heterojunction for efficient CO_(2)-to-C_(2)H_(6)photoconversion.The C_(2)H_(6)production rate reached 167.1µmol g^(-1)h^(-1)with the electron selectivity of 81.1%in the absence of any sacrificial agents.The spectroscopic characterizations indicated that BiOCl nanosheets,acting as the charge relay,directionally transferred the photogenerated electrons from itself and CuBi2O4 nanorods to PdNPs for C-C coupling.The coordinated ensemble of PdNPs and heterojunction significantly elevated the charge separation and transfer efficiency.Moreover,the in-situ spectroscopic analysis supported by theoretical simulations demonstrated that the electron-rich PdNPs generated by the charge relay of PdNPs and heterojunction optimized the CO_(2)-to-C_(2)H_(6)reaction pathway and reduced the energy barrier of the key*CHOCO intermediates.This work develops an innovative strategy to design the multifunctional catalysts for the photoconversion of CO_(2)to value-added carbon products.展开更多
基金supported by the National Natural Science Foundation of China(22302002,22375006)the University Science Research Project of Anhui Province(2022AH050182,2022AH020020)。
文摘Solar-driven CO_(2)conversion to prepare value-added products is highly desirable but challenging.Central to the achievement of multi-carbon products via CO_(2)photoconversion is to break the bottlenecks of C-C coupling and multi-electron transfer.Herein,a charge relay system consisting of Pd-decorated BiOCl-wrapped CuBi_(2)O_(4)is reported by taking advantage of the synergy of Pd nanoparticles(PdNPs)and heterojunction for efficient CO_(2)-to-C_(2)H_(6)photoconversion.The C_(2)H_(6)production rate reached 167.1µmol g^(-1)h^(-1)with the electron selectivity of 81.1%in the absence of any sacrificial agents.The spectroscopic characterizations indicated that BiOCl nanosheets,acting as the charge relay,directionally transferred the photogenerated electrons from itself and CuBi2O4 nanorods to PdNPs for C-C coupling.The coordinated ensemble of PdNPs and heterojunction significantly elevated the charge separation and transfer efficiency.Moreover,the in-situ spectroscopic analysis supported by theoretical simulations demonstrated that the electron-rich PdNPs generated by the charge relay of PdNPs and heterojunction optimized the CO_(2)-to-C_(2)H_(6)reaction pathway and reduced the energy barrier of the key*CHOCO intermediates.This work develops an innovative strategy to design the multifunctional catalysts for the photoconversion of CO_(2)to value-added carbon products.
