Di Yuqian, Li Huaxin, Yu Xianbo, Chen Hu, Xie Shuao, Xi Xiaoxue, Han Wei, Hu Zhongbo, Yue Xian, Xiang Junhui
Center of Materials Science and Optoelectronics Engineering, College of Materials Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
International College, University of Chinese Academy of Sciences, Beijing 100049, China.
J Colloid Interface Sci. 2025 Nov 15;698:138031. doi: 10.1016/j.jcis.2025.138031. Epub 2025 May 30.
The exceptional photovoltaic properties of graphitic carbon nitride, g-CN (CN), make it a promising candidate for advancing artificial photosynthesis, particularly in the area of photocatalytic CO reduction. However, limited catalytically active sites and inefficient separation of charge carriers significantly hinder CN's CO photocatalytic activity and efficiency. In this study, a star-shaped Fe(PO)(OH) (FeP)/CN heterojunction photocatalyst was designed and synthesized for high-efficiency photocatalytic CO reduction. The FeP compounds are chemically anchored to the surface of CN nanosheets, forming an electron transfer channel between FeP and CN. Here, a resulting FeP/CN photocatalyst exhibited spatial separation of photogenerated carriers and achieved a remarkable conversion rate of 62.63 μmol/g under CO conditions with only 2 mL of CO and without a sacrificial agent. Compared with pure CN and FeP, the photocatalytic activity increased by 3.50 times and 5.20 times, respectively. Density functional theory calculations indicate the Gibbs free energy of the key intermediate *COOH at the FeP/CN interface is significantly lowered compared to CN, enhancing its photocatalytic performance. This study proposes an innovative strategy for metal- and submetal-doped CN-based photocatalysts and provides insights into the photoconversion of CO at room temperature and pressure, without sacrificial agents.
石墨相氮化碳（g-CN，简称CN）优异的光伏特性使其成为推进人工光合作用的有前途的候选材料，特别是在光催化CO还原领域。然而，有限的催化活性位点和电荷载流子的低效分离显著阻碍了CN的CO光催化活性和效率。在本研究中，设计并合成了一种星形Fe(PO)(OH)（FeP）/CN异质结光催化剂用于高效光催化CO还原。FeP化合物化学锚定在CN纳米片表面，在FeP和CN之间形成电子转移通道。在此，所得的FeP/CN光催化剂表现出光生载流子的空间分离，在仅2 mL CO且无牺牲剂的CO条件下实现了62.63 μmol/g的显著转化率。与纯CN和FeP相比，光催化活性分别提高了3.50倍和5.20倍。密度泛函理论计算表明，与CN相比，FeP/CN界面处关键中间体*COOH的吉布斯自由能显著降低，增强了其光催化性能。本研究提出了一种基于金属和亚金属掺杂的CN基光催化剂的创新策略，并为在室温和常压下无牺牲剂的CO光转化提供了见解。
