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

Science China Materials 2022年第5期65卷 1252-1261页

作者： Yang Lv Xin Mao Wanbing Gong Dongdong Wang Chun Chen Porun Liu Yue Lin Guozhong Wang Haimin Zhang Aijun Du Huijun Zhao Key Laboratory of Materials Physics Centre 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 Chemistry Physics and Mechanical EngineeringScience and Engineering FacultyQueensland University of TechnologyGardens Point CampusBrisbaneQLD 4001Australia Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China Centre for Catalysis and Clean Energy Griffith UniversityGold Coast CampusQueensland 4222Australia

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.

关键词： crystal phase engineering hcp-phased ni nanoparticles catalytic hydrogenation DFT calculations H_(2)O solvent

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