Controlling efficient interfacial charge transfer is crucial for developing advanced photocatalysts.This study successfully developed a bifunctional photocatalyst with an S-scheme heterojunction by incorporating ReS_(...Controlling efficient interfacial charge transfer is crucial for developing advanced photocatalysts.This study successfully developed a bifunctional photocatalyst with an S-scheme heterojunction by incorporating ReS_(2) into the Zn_(3)In_(2)S_(6)(ZIS)nanoflower structure,enabling the organic pollutants degradation and synergistic hydrogen production.The optimized ZIS/ReS_(2)-1%exhibited exceptional photocatalytic efficiency,reaching a 97.7%degradation rate of ibuprofen(IBP)within 2 h,along with a hydrogen generation rate of 1.84 mmol/g/h.The degradation efficiency and hydrogen generation rate were 1.78 and 5.75 times greater than those of Zn_(3)In_(2)S_(6),respectively.Moreover,ZIS/ReS_(2)-1%demonstrated excellent catalytic degradation abilities for various organic pollutants such as ciprofloxacin,amoxicillin,norfloxacin,levofloxacin,ofloxacin,sulfamethoxazole,and tetracycline,while also showing good synergistic hydrogen production efficiency.Electron spin resonance and radical scavenging experiments verified that h+,·O^(2)-,and @·OH were the primary reactive species responsible for IBP degradation.The superior photocatalytic performance of the ZIS/ReS_(2)-1%was mainly attributed to its broad and intense absorption of visible light,effective separation of charge carriers,and enhanced redox capabilities.The degradation pathway of IBP was unveiled through Fukui function and liquid chromatography-mass spectrometry,and the toxicity of the degradation intermediates was also examined.In-situ XPS and density functional theory(DFT)calculations confirmed the existence of S-scheme heterojunction.This study provided a new pathway for simultaneously achieving organic pollutant treatment and energy conversion.展开更多
By harnessing the power of MoS_(2) as a cocatalyst to enhance electron transfer and charge carrier separation,a groundbreaking two-in-one redox photocatalytic system was developed.This innovative system integrated 2D ...By harnessing the power of MoS_(2) as a cocatalyst to enhance electron transfer and charge carrier separation,a groundbreaking two-in-one redox photocatalytic system was developed.This innovative system integrated 2D MoS_(2) nanosheets onto hydrangea-like Zn_(3)In_(2)S_(6) nanosheets,forming a 2D/3D heterostructure that established a stable and intimate interface.This unique architecture significantly improved cooperative photocatalytic performance,enabling the simultaneous production of hydrogen and benzaldehyde under light irradiation≥420 nm.Notably,the system achieved remarkable yields of hydrogen(41.9 mmol g^(-1) h^(-1))and benzaldehyde(38.9 mmol g^(-1) h^(-1)),surpassing the pristine Zn_(3)In_(2)S_(6) by 22.4 times.An impressive electron-hole pair utilization rate of approximately 93%was attained,underscoring the high efficiency of this two-in-one redox system.Additionally,the targeted 10 wt%-MoS_(2) loaded Zn_(3)In_(2)S_(6)(10MZ)nanohybrids at 400 nm obtained an apparent quantum yield(AQY)value of 17.66%without sacrificial agents or noble metals.The exceptional performance was attributed to improved charge carrier separation and reduced recombination,facilitated by cocatalyst integration and evidenced via photoluminescence,photoelectrochemical and Kelvin probe force microscopy measurements.This work highlighted the critical role of two-in-one redox-functioning heterojunctions in optimizing electron-hole pair utilization,offering a promising approach for sustainable energy production and organic synthesis.By demonstrating the potential for efficient,simultaneous generation of valuable chemicals and fuels,this research paves the way for the development of next-generation photocatalytic systems.展开更多
基金financially supported by ‘14th Five Years Plan-Systematic Evaluation of Carbon Footprint and Environmental Safety of Bamboo-based Plastic Substitute Products (Grant No. 2023YFD2202105)’‘14th Five Years Plan-Key Technology of Conversing Bamboo Wastes to New Carbonbased Materials (Grant No. 2022YFD2200904)’+2 种基金‘Basic Scientific Research Funds of International Centre for Bamboo and Rattan (Grant No. 1632023003)’‘Science and Technology Planning Project of Nanping City (Grant No. N2022B007)’financial support from the China Scholarship Council.
文摘Controlling efficient interfacial charge transfer is crucial for developing advanced photocatalysts.This study successfully developed a bifunctional photocatalyst with an S-scheme heterojunction by incorporating ReS_(2) into the Zn_(3)In_(2)S_(6)(ZIS)nanoflower structure,enabling the organic pollutants degradation and synergistic hydrogen production.The optimized ZIS/ReS_(2)-1%exhibited exceptional photocatalytic efficiency,reaching a 97.7%degradation rate of ibuprofen(IBP)within 2 h,along with a hydrogen generation rate of 1.84 mmol/g/h.The degradation efficiency and hydrogen generation rate were 1.78 and 5.75 times greater than those of Zn_(3)In_(2)S_(6),respectively.Moreover,ZIS/ReS_(2)-1%demonstrated excellent catalytic degradation abilities for various organic pollutants such as ciprofloxacin,amoxicillin,norfloxacin,levofloxacin,ofloxacin,sulfamethoxazole,and tetracycline,while also showing good synergistic hydrogen production efficiency.Electron spin resonance and radical scavenging experiments verified that h+,·O^(2)-,and @·OH were the primary reactive species responsible for IBP degradation.The superior photocatalytic performance of the ZIS/ReS_(2)-1%was mainly attributed to its broad and intense absorption of visible light,effective separation of charge carriers,and enhanced redox capabilities.The degradation pathway of IBP was unveiled through Fukui function and liquid chromatography-mass spectrometry,and the toxicity of the degradation intermediates was also examined.In-situ XPS and density functional theory(DFT)calculations confirmed the existence of S-scheme heterojunction.This study provided a new pathway for simultaneously achieving organic pollutant treatment and energy conversion.
基金support provided by the Ministry of Higher Education Malaysia under the Xiamen University Malaysia.-Fundamental Research Grant Scheme(FRGS)(Ref no.FRGS/1/2024/TK08/XMU/02/1)supported by the PETRONAS-Academia Collaboration Dialogue(PACD 2023)grant,provided by PETRONAS Research Sdn.Bhd.(PRSB)+6 种基金the Ministry of Science,Technology and Innovation(MOSTI)Malaysia under the Strategic Research Fund(SRF)(S.22015)supported by the National Natural Science Foundation of China(Ref no:22202168)Guangdong Basic and Applied Basic Research Foundation(Ref no:2021A1515111019)the financial support from the State Key Laboratory of Physical Chemistry of Solid Surfaces,Xiamen University(Ref no:2023X11)supported by the Xiamen University,Embassy of the People's Republic of China in Malaysia(EENG/0045)funded by Xiamen University Malaysia Investigatorship Grant(Grant no:IENG/0038)Xiamen University Malaysia Research Fund(ICOE/0001,XMUMRF/2021-C8/IENG/0041 and XMUMRF/2025-C15/IENG/0080).
文摘By harnessing the power of MoS_(2) as a cocatalyst to enhance electron transfer and charge carrier separation,a groundbreaking two-in-one redox photocatalytic system was developed.This innovative system integrated 2D MoS_(2) nanosheets onto hydrangea-like Zn_(3)In_(2)S_(6) nanosheets,forming a 2D/3D heterostructure that established a stable and intimate interface.This unique architecture significantly improved cooperative photocatalytic performance,enabling the simultaneous production of hydrogen and benzaldehyde under light irradiation≥420 nm.Notably,the system achieved remarkable yields of hydrogen(41.9 mmol g^(-1) h^(-1))and benzaldehyde(38.9 mmol g^(-1) h^(-1)),surpassing the pristine Zn_(3)In_(2)S_(6) by 22.4 times.An impressive electron-hole pair utilization rate of approximately 93%was attained,underscoring the high efficiency of this two-in-one redox system.Additionally,the targeted 10 wt%-MoS_(2) loaded Zn_(3)In_(2)S_(6)(10MZ)nanohybrids at 400 nm obtained an apparent quantum yield(AQY)value of 17.66%without sacrificial agents or noble metals.The exceptional performance was attributed to improved charge carrier separation and reduced recombination,facilitated by cocatalyst integration and evidenced via photoluminescence,photoelectrochemical and Kelvin probe force microscopy measurements.This work highlighted the critical role of two-in-one redox-functioning heterojunctions in optimizing electron-hole pair utilization,offering a promising approach for sustainable energy production and organic synthesis.By demonstrating the potential for efficient,simultaneous generation of valuable chemicals and fuels,this research paves the way for the development of next-generation photocatalytic systems.
