Tandem synthesis of tertiary amines using graphene encapsulated Ni nocatalyst via nitro compounds hydrogenation and primary amine methylation

作     者：Jianguo Liu Yanpei Song Huanli Wang Longlong Ma Jianguo Liu;Yanpei Song;Huanli Wang;Longlong Ma

作者机构：Key Laboratory of Energy Thermal Conversion and Control of Ministry of EducationSchool of Energy and EnvironmentSoutheast UniversityNanjing210096China Dalian National Laboratory for Clean EnergyDalian116023China CAS Key Laboratory of Renewable EnergyGuangdong Provincial Key Laboratory of New and Renewable Energy Research and DevelopmentGuangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou510640China 

出 版 物：《Green Chemical Engineering》 (绿色化学工程（英文）)

年 卷 期：2022年第3卷第1期

页      面：64-70页

核心收录：

学科分类：07[理学] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 070303[理学-有机化学] 0703[理学-化学] 

基　　金：National Key R&D Program of China(2019YFD1100601) National Natural Science Foundation of China(Project 51976225) Dalian National Laboratory Cooperation Foundation,Chinese Academy of Sciences(Project DNL201916)for financial support。 

主　　题：Encapsulated graphene shell Ni@graphene catalyst Selective hydrogenation Nitro compounds 

摘      要：Development of the economic, environmentally friendly synthesis of amines from nitro compounds remains important and challenging. In this work, the graphene shell encapsulated none noble Ni-based catalysts were successfully designed and synthesized via an environmentally friendly method using H2O or Et OH as solvent. These fresh and recycling catalysts were characterized by X-ray diffraction and X-ray photoelectron spectroscopy. For the nitro compounds hydrogenation, Ni@C-600-H2O exhibits the best catalytic activity to achieve 100 mol/mol conversions of nitrobenzene and 99% selectivity of aniline under mild reaction conditions of 1.0 MPa H2and 60°C.Many halogen-substituted, olefin substituted nitro compounds and aliphatic nitro compounds were investigated and desired products were obtained in excellent selectivity. What is more, the catalyst had excellent stability and could be recycled 13 times without any significant loss in selectivity and activity. Furthermore, we also reported the methodology for tertiary amines synthesis using Ni-based catalyst via one-pot, cost-effective tandem combination reaction with nitrobenzene hydrogenation and amines N-methylation.