Wang Yu, Qin Ruixuan, Wang Yongke, Ren Juan, Zhou Wenting, Li Laiyang, Ming Jiang, Zhang Wuyong, Fu Gang, Zheng Nanfeng
State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National & Local Joint Engineering Research Center of Preparation Technology of Nanomaterials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Angew Chem Int Ed Engl. 2020 Jul 27;59(31):12736-12740. doi: 10.1002/anie.202003651. Epub 2020 May 25.
Catalytic hydrogenation of nitroaromatics is an environment-benign strategy to produce industrially important aniline intermediates. Herein, we report that Fe(OH) deposition on Pt nanocrystals to give Fe(OH) /Pt, enables the selective hydrogenation of nitro groups into amino groups without hydrogenating other functional groups on the aromatic ring. The unique catalytic behavior is identified to be associated with the Fe -OH-Pt interfaces. While H activation occurs on exposed Pt atoms to ensure the high activity, the high selectivity towards the production of substituted aniline originates from the Fe -OH-Pt interfaces. In situ IR, X-ray photoelectron spectroscopy (XPS), and isotope effect studies reveal that the Fe /Fe redox couple facilitates the hydrodeoxygenation of the -NO group during hydrogenation catalysis. Benefitting from Fe -OH-Pt interfaces, the Fe(OH) /Pt catalysts exhibit high catalytic performance towards a broad range of substituted nitroarenes.
硝基芳烃的催化氢化是一种环境友好型策略，用于生产具有重要工业价值的苯胺中间体。在此，我们报道在铂纳米晶体上沉积氢氧化铁得到Fe(OH)/Pt，能够将硝基选择性氢化成氨基，而不会氢化芳环上的其他官能团。独特的催化行为被确定与Fe-OH-Pt界面有关。虽然H活化发生在暴露的Pt原子上以确保高活性，但对取代苯胺生产的高选择性源于Fe-OH-Pt界面。原位红外光谱、X射线光电子能谱(XPS)和同位素效应研究表明，Fe/Fe氧化还原对在氢化催化过程中促进了-NO基团的加氢脱氧。受益于Fe-OH-Pt界面，Fe(OH)/Pt催化剂对多种取代硝基芳烃表现出高催化性能。
