hcp-phased Ni nanoparticles with generic catalytic hydrogenation activities toward different functional groups

作     者：Yang Lv Xin Mao Wanbing Gong Dongdong Wang Chun Chen Porun Liu Yue Lin Guozhong Wang Haimin Zhang Aijun Du Huijun Zhao 吕扬;冒鑫;龚万兵;汪东东;陈春;刘珀润;林岳;汪国忠;张海民;杜爱军;赵惠军

作者机构：Key Laboratory of Materials PhysicsCentre for Environmental and Energy NanomaterialsAnhui Key Laboratory of Nanomaterials and NanotechnologyInstitute of Solid State PhysicsHefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China School of ChemistryPhysics and Mechanical EngineeringScience and Engineering FacultyQueensland University of TechnologyGardens Point CampusBrisbaneQLD 4001Australia Hefei National Laboratory for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei 230026China Centre for Catalysis and Clean EnergyGriffith UniversityGold Coast CampusQueensland 4222Australia 

出 版 物：《Science China Materials》 (中国科学（材料科学（英文版）)

年 卷 期：2022年第65卷第5期

页      面：1252-1261页

核心收录：

学科分类：081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 0702[理学-物理学] 

基　　金：financially supported by the National Natural Science Foundation of China (51902311 and 51871209) 

主　　题：crystal phase engineering hcp-phased Ni nanoparticles catalytic hydrogenation DFT calculations H_(2)O solvent 

摘      要：Catalytic hydrogenation is a vital industrial means to produce value-added fuels and fine chemicals,however, requiring highly efficient catalysts, especially the nonprecious ones. To date, the majority of high-performance industrial hydrogenation catalysts are made of precious metals-based materials, and any given catalyst could only be used to catalyze one or few specific reactions. Herein, we exemplify a crystal phase engineering approach to empower Ni nanoparticles(NPs) with superb intrinsic catalytic activities toward a wide spectrum of hydrogenation reactions. A facile pyrolysis approach is used to directly convert a Ni-imidazole MOF precursor into hexagonal close-packed(hcp)-phased Ni NPs on carbon support. The as-synthesized hcp-phased Ni NPs exhibit unprecedented hydrogenation catalytic activities in pure water towards nitro-, aldehyde-, ketone-, alkene-and N heterocyclic-compounds, outperforming the face-centered cubic(fcc)-Ni counterpart and the reported transition metalsbased catalysts. The density functional theory calculations unveil that the presence of hcp-Ni boosts the intrinsic catalytic hydrogenation activity by coherently enhancing the substrate adsorption strength and lowering the reaction barrier energy of the rate-determining step. We anticipate that the crystal phase engineering design approach unveiled in this work would be adoptable to other types of reactions.