Hu Haijun, Sun Xiaodong, Li Hui, Pan Hongge, Ma Yali, Huang Hongwei, Ma Tianyi
Institute of Clean Energy Chemistry, Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials, College of Chemistry, Liaoning University, Shenyang, 110036, P. R. China.
Centre for Atomaterials and Nanomanufacturing (CAN), School of Science, RMIT University, Melbourne, VIC, 3000, Australia.
Small. 2025 Jan;21(2):e2407117. doi: 10.1002/smll.202407117. Epub 2024 Nov 7.
Due to the severe recombination of charge carriers, the photocatalytic activity of covalent organic frameworks (COFs) materials is limited. Herein, through simple ultrasound and stirring processes, the Pd metallene (Pde) is successfully combined with 2D COFs to form Pde/TpPa-1-COF (Pde/TPC) composites. Obviously, a strong internal electric field (IEF) is successfully formed in Pde/TPC hybrid materials, which significantly boosts the separation of photogenerated charges. In addition, the matched 2D structure of the two materials can also lead to electronic coupling effects, plentiful active sites, and shortened carrier migration paths. Thus, the Pde/TPC hybrid materials own extraordinary carrier separation ability with a longer carriers lifetime (3.3 ns for Pde/TPC and 2.7 ns for TPC), which can be proved series of photoelectrochemical and spectroscopic tests. Benefiting from the formation of IEF and the matched 2D structure, the 8% Pde/TPC demonstrates the highest photocatalytic H evolution efficiency, with H production rate reaching up to 5.85 mmol g h, which is over 25 times greater than that of pristine COFs, also exceeding that of many reported COFs-based photocatalysts. This research provides new perspectives and innovative approaches to further research on enhancing the internal electric field of COFs to promote their photocatalytic performance.
由于电荷载流子的严重复合，共价有机框架（COFs）材料的光催化活性受到限制。在此，通过简单的超声和搅拌过程，成功地将钯金属烯（Pde）与二维COFs结合，形成Pde/TpPa-1-COF（Pde/TPC）复合材料。显然，在Pde/TPC杂化材料中成功形成了强内电场（IEF），这显著促进了光生电荷的分离。此外，两种材料匹配的二维结构还可导致电子耦合效应、丰富的活性位点以及缩短的载流子迁移路径。因此，Pde/TPC杂化材料具有非凡的载流子分离能力，载流子寿命更长（Pde/TPC为3.3 ns，TPC为2.7 ns），这可通过一系列光电化学和光谱测试得到证明。得益于IEF的形成和匹配的二维结构，8%的Pde/TPC表现出最高的光催化析氢效率，产氢速率高达5.85 mmol g h，这比原始COFs高出25倍以上，也超过了许多已报道的基于COFs的光催化剂。该研究为进一步研究增强COFs的内电场以提高其光催化性能提供了新的视角和创新方法。
