School of Chemistry and Chemical Engineering, Hefei University of Technology, Hefei, Anhui230009, China.
Anhui Province Key Laboratory of Advance Catalytic Materials and Reaction Engineering, Hefei230009, P. R. China.
ACS Appl Mater Interfaces. 2023 Jan 25;15(3):4845-4856. doi: 10.1021/acsami.2c22686. Epub 2023 Jan 11.
Selective reduction of nitroaromatics to the corresponding amines generally requires complex conditions, involving pressurized hydrogen, higher temperatures, or organic acids. In this work, we successfully prepared a series of porphyrin-based MOF photocatalysts (Pd-PMOFs, In-PMOFs, and In/Pd-PMOFs) via a facile solvothermal method for the efficient selective reduction of nitroaromatics to corresponding anilines with deionized water as the hydrogen donor. Being a new structured material (monoclinic, CHInNOPd), on account of the abundant pore channels, strong light absorption capability, well-matched bandgap, as well as the coordination of indium ions and palladium ions, In/Pd-MOFs have excellent migration efficiency of photo-induced electrons and holes. Specifically, the In/Pd-PMOF photocatalyst manifested superior conversion (100%) and selectivity (≥80%) toward the screened nitro compounds under mild conditions. This work avoids the use of strong reductants, organic acids, and pressurized hydrogen gas as hydrogen sources, providing a promising concept for developing green catalytic systems.
将硝基芳烃选择性还原为相应的胺通常需要复杂的条件,涉及加压氢气、较高的温度或有机酸。在这项工作中,我们通过简便的溶剂热法成功制备了一系列基于卟啉的 MOF 光催化剂(Pd-PMOFs、In-PMOFs 和 In/Pd-PMOFs),可在去离子水作为供氢体的条件下高效选择性还原硝基芳烃为相应的苯胺。作为一种新型结构材料(单斜晶系,CHInNOPd),由于丰富的孔道、较强的光吸收能力、匹配的能带隙以及铟离子和钯离子的配位作用,In/Pd-MOFs 具有优异的光生电子和空穴迁移效率。具体来说,In/Pd-PMOF 光催化剂在温和条件下对筛选出的硝基化合物表现出优异的转化率(100%)和选择性(≥80%)。这项工作避免了使用强还原剂、有机酸和加压氢气作为氢源,为开发绿色催化体系提供了有前景的概念。