Solar-powered H_(2)O_(2)synthesis from water and oxygen presents a potential strategy in the industrial and environmental domains.However,insufficient light absorption,poor charge separation efficiency,and the same or...Solar-powered H_(2)O_(2)synthesis from water and oxygen presents a potential strategy in the industrial and environmental domains.However,insufficient light absorption,poor charge separation efficiency,and the same or nearby catalytic sites for the photocatalysts limit the activity of H_(2)O_(2)production.Herein,an ultraviolet-visible-near-infrared light responsive S-scheme heterojunction is created by growing ZnIn_(2)S_(4)(ZIS)subunits firmly on a core of resorcinol-formaldehyde(RF)sphere.The enhanced full-spectrum light response ZIS/RF core-shell structure is evidenced by UV/Vis-NIR diffuse reflectance spectra(DRS).In situ irradiation X-ray photoelectron spectroscopy(XPS)investigation confirms an S-scheme charge transfer mechanism between RF and ZIS.A directional interfacial electric field(IEF)drives the unique spatial separation feature of constructed heterojunction photoexcited carriers and redox centers through the S-scheme transfer pathway with H_(2)O_(2)production.Under solar light irradiation,the optimized ZIS/RF with core-shell structure shows a robust apparent quantum efficiency(AQY)up to 22.5%at 420 nm,1%at 720 nm,and 0.2%at 800 nm.With the key reaction intermediates determined by calculating the average number of transferred electrons and oxygen-reactive species,a possible full-spectrum-light-driven redox mechanism of H_(2)O_(2)synthesis is provided.展开更多
基金supported by the General Research Fund(No.18300920)of Research Grants Council,Hong Kong,Dean’s Research Fund(Nos.04638 and C3688),FLASS,EdUHKMulti-disciplinary Research Capacity Building Scheme(No.04A29)EdUHK,Scientific Research Startup Foundation of Jiangsu Univer-sity(No.22JDG020).
文摘Solar-powered H_(2)O_(2)synthesis from water and oxygen presents a potential strategy in the industrial and environmental domains.However,insufficient light absorption,poor charge separation efficiency,and the same or nearby catalytic sites for the photocatalysts limit the activity of H_(2)O_(2)production.Herein,an ultraviolet-visible-near-infrared light responsive S-scheme heterojunction is created by growing ZnIn_(2)S_(4)(ZIS)subunits firmly on a core of resorcinol-formaldehyde(RF)sphere.The enhanced full-spectrum light response ZIS/RF core-shell structure is evidenced by UV/Vis-NIR diffuse reflectance spectra(DRS).In situ irradiation X-ray photoelectron spectroscopy(XPS)investigation confirms an S-scheme charge transfer mechanism between RF and ZIS.A directional interfacial electric field(IEF)drives the unique spatial separation feature of constructed heterojunction photoexcited carriers and redox centers through the S-scheme transfer pathway with H_(2)O_(2)production.Under solar light irradiation,the optimized ZIS/RF with core-shell structure shows a robust apparent quantum efficiency(AQY)up to 22.5%at 420 nm,1%at 720 nm,and 0.2%at 800 nm.With the key reaction intermediates determined by calculating the average number of transferred electrons and oxygen-reactive species,a possible full-spectrum-light-driven redox mechanism of H_(2)O_(2)synthesis is provided.
