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Verifying the Unique Charge Migration Pathway in Polymeric Homojunctions for Artificial Photosynthesis of Hydrogen Peroxide

Qiang ChengCollege of Urban and Environmental Sciences Hubei Key Laboratory of Pollutant Analysis and Reuse Technology Hubei Normal University Huangshi 435002 P. R. ChinaJingping LiCollege of Urban and Environmental Sciences Hubei Key Laboratory of Pollutant Analysis and Reuse Technology Hubei Normal University Huangshi 435002 P. R. ChinaYuxin HuangCollege of Urban and Environmental Sciences Hubei Key Laboratory of Pollutant Analysis and Reuse Technology Hubei Normal University Huangshi 435002 P. R. ChinaXiufan LiuCollege of Urban and Environmental Sciences Hubei Key Laboratory of Pollutant Analysis and Reuse Technology Hubei Normal University Huangshi 435002 P. R. ChinaBiao ZhouCollege of Urban and Environmental Sciences Hubei Key Laboratory of Pollutant Analysis and Reuse Technology Hubei Normal University Huangshi 435002 P. R. ChinaQiao XiongCollege of Urban and Environmental Sciences Hubei Key Laboratory of Pollutant Analysis and Reuse Technology Hubei Normal University Huangshi 435002 P. R. ChinaKai WangCollege of Urban and Environmental Sciences Hubei Key Laboratory of Pollutant Analysis and Reuse Technology Hubei Normal University Huangshi 435002 P. R. China
2025en
ABI

Abstract

Abstract Artificial photosynthesis for producing high‐value hydrogen peroxide (H 2 O 2 ) using carbon nitride‐based systems holds immense potential. However, understanding the charge transfer dynamics in homojunction photocatalysts remains a significant challenge owing to the limitations of current characterization techniques. Here, a polymeric C 3 N 5 /C 3 N 4 homojunction (CNHJ) is employed as a model system to probe interfacial electron transfer. Bimetallic cocatalysts serve as sensitive probes, enabling in situ tracking of the S‐scheme electron transfer between C 3 N 5 and C 3 N 4 via X‐ray photoelectron spectroscopy. Leveraging the unique advantages of this S‐scheme, the CNHJ demonstrates substantially enhanced performance in the two‐electron oxygen reduction reaction, achieving an impressive H 2 O 2 production rate of 8.78 mmol g −1 h −1 under visible light irradiation. Furthermore, the system demonstrates robust performance in continuous‐flow setups, under natural sunlight, and in photocatalytic disinfection tests, highlighting its practical potential. This approach offers new insights into dynamic electron transfer mechanisms and paves the way for advancing artificial photosynthesis technologies.

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