摘要
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.
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)
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)。
