Broad absorption spectra with efficient generation and separation of available charge carriers are indispensable requirements for promising semiconductor-based photocatalysts to achieve the ultimate goal of solar-to-f...Broad absorption spectra with efficient generation and separation of available charge carriers are indispensable requirements for promising semiconductor-based photocatalysts to achieve the ultimate goal of solar-to-fuel conversion.Here,Cu_(3-x)SnS_(4)(x=0-0.8)with copper vacancies have been prepared and fabricated via solvothermal process.The obtained copper vacancy materials have extended light absorption from ultraviolet to near-infrared-II region for its significant plasmonic effects.Time-resolved photoluminescence shows that the vacancies can simultaneously optimize charge carrier dynamics to boost the generation of long-lived active electrons for photocatalytic reduction.Density functional theory calculations and electrochemical characterizations further revealed that copper vacancies in Cu_(3-x)SnS_(4)tend to enhance hydrogen’s adsorption energy with an obvious decrease in its H_(2)evolution reaction(HER)overpotential.Furthermore,without any loadings,the H_(2)production rate was measured to be 9.5 mmol·h^(-1)·g^(-1).The apparent quantum yield was measured to be 27%for wavelengthλ>380 nm.The solar energy conversion efficiency was measured to be 6.5%under visible-near infrared(vis-NIR)(λ>420 nm).展开更多
基金The work is supported by the Science and Technology Commission of Shanghai Municipality(Nos.19JC1412600,20520741400,and 18230743400)the National Natural Science Foundation of China(Nos.21771124 and 21671134).
文摘Broad absorption spectra with efficient generation and separation of available charge carriers are indispensable requirements for promising semiconductor-based photocatalysts to achieve the ultimate goal of solar-to-fuel conversion.Here,Cu_(3-x)SnS_(4)(x=0-0.8)with copper vacancies have been prepared and fabricated via solvothermal process.The obtained copper vacancy materials have extended light absorption from ultraviolet to near-infrared-II region for its significant plasmonic effects.Time-resolved photoluminescence shows that the vacancies can simultaneously optimize charge carrier dynamics to boost the generation of long-lived active electrons for photocatalytic reduction.Density functional theory calculations and electrochemical characterizations further revealed that copper vacancies in Cu_(3-x)SnS_(4)tend to enhance hydrogen’s adsorption energy with an obvious decrease in its H_(2)evolution reaction(HER)overpotential.Furthermore,without any loadings,the H_(2)production rate was measured to be 9.5 mmol·h^(-1)·g^(-1).The apparent quantum yield was measured to be 27%for wavelengthλ>380 nm.The solar energy conversion efficiency was measured to be 6.5%under visible-near infrared(vis-NIR)(λ>420 nm).
