Cheng Qiang, Li Jingping, Huang Yuxin, Liu Xiufan, Zhou Biao, Xiong Qiao, Wang Kai
College of Urban and Environmental Sciences, Hubei Key Laboratory of Pollutant Analysis and Reuse Technology, Hubei Normal University, Huangshi, 435002, P. R. China.
Adv Sci (Weinh). 2025 Apr;12(16):e2500218. doi: 10.1002/advs.202500218. Epub 2025 Mar 5.
Artificial photosynthesis for producing high-value hydrogen peroxide (HO) 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 CN/CN 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 CN and CN 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 HO production rate of 8.78 mmol g h 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.
利用基于氮化碳的体系通过人工光合作用生产高价值的过氧化氢（HO）具有巨大潜力。然而，由于当前表征技术的局限性，了解同质结光催化剂中的电荷转移动力学仍然是一项重大挑战。在此，采用聚合物CN/CN同质结（CNHJ）作为模型系统来探测界面电子转移。双金属助催化剂作为灵敏探针，能够通过X射线光电子能谱原位追踪CN和CN之间的S型电子转移。利用这种S型的独特优势，CNHJ在两电子氧还原反应中表现出显著增强的性能，在可见光照射下实现了高达8.78 mmol g h的过氧化氢产率。此外，该系统在连续流装置、自然阳光下以及光催化消毒测试中都表现出稳健的性能，突出了其实际应用潜力。这种方法为动态电子转移机制提供了新的见解，并为推进人工光合作用技术铺平了道路。
