The photocatalytic conversion of biomass into high-value chemicals,coupled with simultaneous hydrogen(H_(2))evolution,leveraging the electrons and holes generated by solar energy,holds great promise for addressing ene...The photocatalytic conversion of biomass into high-value chemicals,coupled with simultaneous hydrogen(H_(2))evolution,leveraging the electrons and holes generated by solar energy,holds great promise for addressing energy demands.In this study,we constructed a dual functional photocatalytic system formed by NiS loaded on Ni doped two-dimensional(2D)CdS nanosheet(NiS/Ni-CdSNS)heterostructure for visible-light-driven H_(2)evolution and ethanol oxidation to acetaldehyde.Remarkably,the 2D NiS/NiCdSNS exhibited significant activity and selectivity in both photocatalytic H_(2)evolution and ethanol oxidation,achieving yields of 7.98 mmol g^(-1)h^(-1)for H_(2)and 7.33 mmol g^(-1)h^(-1)for acetaldehyde.The heterogeneous interface of the composite facilitated efficient charge separation,while NiS provided abundant sites for proton reduction,thereby promoting the overall dual-functional photocatalytic activity.Density functional theory calculations further reveal that both Ni doping and NiS loading can reduce the reaction energy barrier of ethanol oxidation of free radicals,and NiS/Ni-CdSNS composite materials exhibit stronger ethanol C-H activation ability to generate key intermediate·CH(OH)CH_(3)on the surface.This work serves as a valuable guide for the rational design of efficient dual functional photocatalytic systems that combine H_(2)evolution with the selective conversion of organic compounds into high-value chemicals.展开更多
基金supported by the National Key R&D Program of China(No.2022YFB1903200)the National Natural Science Foundation of China(Nos.U23A2087,22372137,22102136,22072057,22227802,22172126)+2 种基金the Key Research and Development Program of Guangxi(No.GUIKE AB23026116)the Fundamental Research Funds for the Central Universities(Nos.20720220105,20720232005)the XMU Training Program of Innovation and Enterpreneurship for Undergraduates(Nos.2022Y1132,202310384027)。
文摘The photocatalytic conversion of biomass into high-value chemicals,coupled with simultaneous hydrogen(H_(2))evolution,leveraging the electrons and holes generated by solar energy,holds great promise for addressing energy demands.In this study,we constructed a dual functional photocatalytic system formed by NiS loaded on Ni doped two-dimensional(2D)CdS nanosheet(NiS/Ni-CdSNS)heterostructure for visible-light-driven H_(2)evolution and ethanol oxidation to acetaldehyde.Remarkably,the 2D NiS/NiCdSNS exhibited significant activity and selectivity in both photocatalytic H_(2)evolution and ethanol oxidation,achieving yields of 7.98 mmol g^(-1)h^(-1)for H_(2)and 7.33 mmol g^(-1)h^(-1)for acetaldehyde.The heterogeneous interface of the composite facilitated efficient charge separation,while NiS provided abundant sites for proton reduction,thereby promoting the overall dual-functional photocatalytic activity.Density functional theory calculations further reveal that both Ni doping and NiS loading can reduce the reaction energy barrier of ethanol oxidation of free radicals,and NiS/Ni-CdSNS composite materials exhibit stronger ethanol C-H activation ability to generate key intermediate·CH(OH)CH_(3)on the surface.This work serves as a valuable guide for the rational design of efficient dual functional photocatalytic systems that combine H_(2)evolution with the selective conversion of organic compounds into high-value chemicals.
