Wang Sheng, Li Shihao, Zheng Chenglong, Feng Huiyi, Feng Yi-Si
School of Chemistry and Chemical Engineering, Hefei University of Technology, Hefei, Anhui 230009, China.
Anhui Province Key Laboratory of Advance Catalytic Materials and Reaction Engineering, Hefei 230009, P. R. China.
Inorg Chem. 2024 Jan 8;63(1):554-563. doi: 10.1021/acs.inorgchem.3c03446. Epub 2023 Dec 27.
The meaningful and rational engineering of porphyrin-based catalysts with multimetallic active sites is very attractive toward photocatalytic hydrogen generation from water decomposition. Herein, three metal organic frameworks (MOFs) based on meso-tetrakis(4-carboxylphenyl)porphyrin (TCPP) were successfully constructed under solvothermal conditions. As a novel architectured photocatalyst (triclinic, CHNOPdYb), Pd/Yb-PMOF manifested diverse metal active sites, suitable bandgap positions, prominent visible light-collecting capacity, excellent carrier transfer efficiency, and obvious synergistic effect between ytterbium and palladium ions. Consequently, such a bimetallic MOF exhibited strengthened photocatalytic hydrogen evolution performance. Concretely, its hydrogen generation efficiency was up to 3196.42 μmol g h with 2 wt % Pt as a cocatalyst under visible light illumination. Our work demonstrates a promising strategy for highly efficient visible-light catalysts based on bimetallic-trimmed porphyrin MOFs.
对具有多金属活性位点的卟啉基催化剂进行有意义且合理的工程设计,对于光催化水分解制氢极具吸引力。在此,基于中位四(4 - 羧基苯基)卟啉(TCPP)成功构建了三种金属有机框架(MOF)。作为一种新型结构的光催化剂(三斜晶系,CHNOPdYb),Pd/Yb - PMOF表现出多样的金属活性位点、合适的带隙位置、突出的可见光收集能力、优异的载流子转移效率以及镱离子和钯离子之间明显的协同效应。因此,这种双金属MOF表现出增强的光催化析氢性能。具体而言,在可见光照射下,以2 wt% Pt作为助催化剂时,其产氢效率高达3196.42 μmol g⁻¹ h⁻¹。我们的工作展示了一种基于双金属修饰卟啉MOF的高效可见光催化剂的有前景的策略。