Chen Yongzhi, Guo Yuanyuan, Wang Tie, Ji Sailun, Shao Haipei, Lin Ming, Seki Shu, Yan Ning, Jiang Donglin
Department of Chemistry, Faculty of Science, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore.
School of Science, Beijing University of Posts and Telecommunications, Beijing, 100876, China.
Nat Commun. 2025 Jul 14;16(1):6495. doi: 10.1038/s41467-025-61853-4.
Artificial photosynthesis is impeded by rapid charge recombination and inefficient use of photogenerated carriers. Here we present covalent organic frameworks with systematically tailored skeletons and pores for green yet efficient photosynthesis with water and air. The hexavalent frameworks with non-conjugated photocatalytic skeletons enable water oxidation at knot corners and oxygen reduction at linker edges, while orientated triangular micropores timely supply water and air. Noteworthily, the framework with the highest π density and smallest supermicropores exhibits optimal charge separation and utilization and achieves rapid, efficient and cyclable hydrogen peroxide production in both batch and membrane reactors. Remarkably, the supermicroporous framework instantly removes organic dye contaminants from water and fully degrades these dyes under visible light. Our findings enable a paradigm shift to the systematic design of both electron/hole flow and mass transport for constructing photocatalysts, which are not only scientifically important but also technologically key to shaping sustainable society and future.
人工光合作用受到快速电荷复合和光生载流子利用效率低下的阻碍。在此，我们展示了具有系统定制骨架和孔隙的共价有机框架，用于以水和空气进行绿色且高效的光合作用。具有非共轭光催化骨架的六价框架能够在节点角处实现水氧化，在连接边处实现氧还原，同时定向三角形微孔及时供应水和空气。值得注意的是，具有最高π密度和最小超微孔的框架表现出最佳的电荷分离和利用，并在间歇式和膜反应器中实现了快速、高效且可循环的过氧化氢生产。引人注目的是，超微孔框架能立即从水中去除有机染料污染物，并在可见光下将这些染料完全降解。我们的发现实现了向构建光催化剂的电子/空穴流和质量传输系统设计的范式转变，这不仅在科学上具有重要意义，而且在塑造可持续社会和未来方面也是技术关键。
