Exploring high efficiency S-scheme heterojunction photocatalysts with strong redox ability for removing volatile organic compounds from the air is of great interest and importance.However,how to predict and regulate t...Exploring high efficiency S-scheme heterojunction photocatalysts with strong redox ability for removing volatile organic compounds from the air is of great interest and importance.However,how to predict and regulate the transport of photogenerated carriers in heterojunctions is a great challenge.Here,density functional theory calculations were first used to successfully predict the formation of a CdS quantum dots/InVO_(4)atomic-layer(110)/(110)facet S-scheme heterojunction.Subsequently,a CdS quantum dots/InVO_(4)atomic-layer was synthesized by in-situ loading of CdS quantum dots with(110)facets onto the(110)facets of InVO_(4)atomic-layer.As a result of the deliberately constructed built-in electric field between the adjoining facets,we obtain a remarkably enhanced photocatalytic degradation rate for ethylene.This rate is 13.8 times that of pure CdS and 13.2 times that of pure InVO_(4).In-situ irradiated X-ray photoelectron spectroscopy,photoluminescence and time-resolved photoluminescence measurements were carried out.These experiments validate that the built-in electric field enhanced the dissociation of photoexcited excitons and the separation of free charge carriers,and results in the formation of S-scheme charge transfer pathways.The reaction mechanism of the photocatalytic C_(2)H_(4)oxidation is investigated by in-situ electron paramagnetic resonance.This work provides a mechanistic insight into the construction and optimization of semiconductor heterojunction photocatalysts for application to environmental remediation.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant No.21902046,21801071,12174092,U21A20500)Overseas Expertise Introduction Center for Discipline Innovation(D18025)+3 种基金the Natural Science Foundation of Hubei Provincial(Grant No.2018CFB171)Wuhan Science and Technology Bureau(2020010601012163)Science and Technology Research Project of Hubei Provincial Department of Education(No.D20221001)the open foundation of the State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences
文摘Exploring high efficiency S-scheme heterojunction photocatalysts with strong redox ability for removing volatile organic compounds from the air is of great interest and importance.However,how to predict and regulate the transport of photogenerated carriers in heterojunctions is a great challenge.Here,density functional theory calculations were first used to successfully predict the formation of a CdS quantum dots/InVO_(4)atomic-layer(110)/(110)facet S-scheme heterojunction.Subsequently,a CdS quantum dots/InVO_(4)atomic-layer was synthesized by in-situ loading of CdS quantum dots with(110)facets onto the(110)facets of InVO_(4)atomic-layer.As a result of the deliberately constructed built-in electric field between the adjoining facets,we obtain a remarkably enhanced photocatalytic degradation rate for ethylene.This rate is 13.8 times that of pure CdS and 13.2 times that of pure InVO_(4).In-situ irradiated X-ray photoelectron spectroscopy,photoluminescence and time-resolved photoluminescence measurements were carried out.These experiments validate that the built-in electric field enhanced the dissociation of photoexcited excitons and the separation of free charge carriers,and results in the formation of S-scheme charge transfer pathways.The reaction mechanism of the photocatalytic C_(2)H_(4)oxidation is investigated by in-situ electron paramagnetic resonance.This work provides a mechanistic insight into the construction and optimization of semiconductor heterojunction photocatalysts for application to environmental remediation.
