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
Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides.Leveraging intrinsic heptazine/triazine phase and face-to-face conta...Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides.Leveraging intrinsic heptazine/triazine phase and face-to-face contact,crystalline C_(3)N_(5)(CC3N5)was combined with protonated g-C_(3)N_(4)(pgCN)through electrostatic self-assembly to achieve robust 2D/2D homojunction interfaces.The highest photocatalytic performance was obtained through crystallinity and homojunction engineering,by controlling the pgCN:CC3N5 ratio.The 25:100 pgCN:CC3N5 homo-junction(25CgCN)had the highest hydrogen production(1409.51 μmol h^(-1))and apparent quantum efficiency(25.04%,420 nm),8-fold and 180-fold higher than CC3N5 and pgCN,respectively.This photocatalytic homojunction improves benzaldehyde and hydrogen production activity,retaining 89%performance after 3 cycles(12 h)on a 3D-printed substrate.Electron paramagnetic resonance demonstrated higher·OH,·O_(2) and hole production of irradiated 25CgCN,attributed to crystallinity and homojunction interaction.Thus,electrostatic self-assembly to couple CC3N5 and pgCN in a 2D/2D homojunction interface ameliorates the performance of multifunctional solar-driven applications.展开更多
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.
基金the financial support provided by the Ministry of Higher Education(MOHE)Malaysia under the Fundamental Research Grant Scheme(FRGS)(Ref no:FRGS/1/2020/TK0/XMU/02/1)The authors would like to thank the Ministry of Science,Technology and Innovation(MOSTI)Malaysia under the Strategic Research Fund(SRF-APP NanoMalaysia BICEP Project 4,S.22015)+5 种基金The authors gratefully acknowledge Agilent Technologies Malaysia Sdn.Bhd.for their contribution through chromatography.This research was supported by the National Natural Science Foundation of China(Ref no:22202168)Guangdong Basic and Applied Basic Research Foundation(Ref no:2021A1515111019)We would also like to acknowledge the financial support from the State Key Laboratory of Physical Chemistry of Solid Surfaces,Xiamen University(Ref.no:2023X11)The authors are thankful to the Embassy of the People's Republic of China in Malaysia for the financial support(Grant no:EENG/0045)This work was also funded by Xiamen University Malaysia Investigatorship Grant(Grant no:IENG/0038)Xiamen University Malaysia Research Fund(ICOE/0001 and XMUMRF/2021-C8/IENG/0041).
文摘Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides.Leveraging intrinsic heptazine/triazine phase and face-to-face contact,crystalline C_(3)N_(5)(CC3N5)was combined with protonated g-C_(3)N_(4)(pgCN)through electrostatic self-assembly to achieve robust 2D/2D homojunction interfaces.The highest photocatalytic performance was obtained through crystallinity and homojunction engineering,by controlling the pgCN:CC3N5 ratio.The 25:100 pgCN:CC3N5 homo-junction(25CgCN)had the highest hydrogen production(1409.51 μmol h^(-1))and apparent quantum efficiency(25.04%,420 nm),8-fold and 180-fold higher than CC3N5 and pgCN,respectively.This photocatalytic homojunction improves benzaldehyde and hydrogen production activity,retaining 89%performance after 3 cycles(12 h)on a 3D-printed substrate.Electron paramagnetic resonance demonstrated higher·OH,·O_(2) and hole production of irradiated 25CgCN,attributed to crystallinity and homojunction interaction.Thus,electrostatic self-assembly to couple CC3N5 and pgCN in a 2D/2D homojunction interface ameliorates the performance of multifunctional solar-driven applications.
