Wen Chunxia, Ni Xinyue, Han Mei, Yu Yue, Liu Chuanqiang, Zhang Yuan, Zheng Beining, Feng Shouhua
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin Provincial International Cooperation Key Laboratory of Advanced Inorganic Solid Functional Materials, College of Chemistry, Jilin University, Changchun, Jilin, 130012, P. R. China.
College of Physics, Jilin University, Changchun, 130012, P. R. China.
Adv Sci (Weinh). 2025 Jul;12(25):e2501026. doi: 10.1002/advs.202501026. Epub 2025 Apr 3.
Homogeneous matrix materials are considered to be a solid guarantee of site-point charge transfer reactions because they are the main body of light absorption, photogenerated carrier separation, migration, and recombination processes. Elucidating the effect of carrier separation efficiency on catalytic performance is of great significance for overcoming the optimization obstacles of homogeneous matrix parts and providing new design strategies. In this study, TiO doped with Fe as the research object quantifies the carrier dynamics while trying to avoid large site and lattice changes. The direct correlation between carrier separation efficiency and photocatalytic performance with different doping content samples is clearly elucidated by carrier dynamic characterization results. Doping of 0.213 wt.% Fe exhibits the best catalytic performance, achieving CO yield of 35.12 µmol g h. Especially, the femtosecond transient absorption spectroscopy demonstrates the defect level formed by doping Fe enhances the separation of photogenerated electrons. The clear relationship shown above, which is catalytic capacity mapping with carrier separation efficiency, rather than a linear dependence on sites and oxygen vacancies, fully demonstrates the great potential of simple doping strategies for homogeneous photocatalysts.
均匀基质材料被认为是位点电荷转移反应的坚实保障，因为它们是光吸收、光生载流子分离、迁移和复合过程的主体。阐明载流子分离效率对催化性能的影响对于克服均匀基质部分的优化障碍并提供新的设计策略具有重要意义。在本研究中，以Fe掺杂的TiO为研究对象，在尽量避免大的位点和晶格变化的同时量化载流子动力学。通过载流子动态表征结果清楚地阐明了不同掺杂含量样品的载流子分离效率与光催化性能之间的直接相关性。0.213 wt.%的Fe掺杂表现出最佳的催化性能，CO产率达到35.12 µmol g h。特别是，飞秒瞬态吸收光谱表明，Fe掺杂形成的缺陷能级增强了光生电子的分离。上述明确的关系，即催化能力与载流子分离效率的映射关系，而不是与位点和氧空位的线性依赖关系，充分证明了简单掺杂策略对均匀光催化剂的巨大潜力。
