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Construction of isolated Ni sites on nitrogen-doped hollow carbon spheres with Ni-N_(3) configuration for enhanced reduction of nitroarenes

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Nano Research 2022年第7期15卷 6001-6009页

作者： Binbin Feng Rou Guo Qiulan Cai Yaping Song Nan Li Yanghe Fu De-Li Chen Jiangwei Zhang Weidong Zhu Fumin Zhang Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China Dalian National Laboratory for Clean Energy&State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Designing and synthesizing high-efficiency non-precious metal-based catalysts having uniform active sites increases the reactivity and selectivity of materials and provides a platform for an in-depth understanding of their catalytic reaction *** this study,we provided an approach for fabricating isolated nickel single-atom sites(Ni SAs)with high loading(4.9 wt.%)stabilized on nitrogen-doped hollow carbon spheres(NHCS)using a core–shell structured Zn/Ni bimetallic zeolitic imidazolate framework(ZIF)composite as the sacrificial *** as-fabricated Ni SAs/NHCS catalyst shows superior activity,selectivity,and recycling durability for the catalytic transfer hydrogenation of nitrobenzene to aniline,thus achieving 100%yield of aniline with a turn-over frequency(TOF)value as high as 29.9 h^(−1) under mild *** TOF value is considerably superior to the supported Ni nanoparticle *** experiments designed show that the hollow structure feature of NHCS facilitates accessible active sites and mass transfer,which thus contributes to the enhancement of the catalytic performance of Ni SAs/*** functional theory calculations show the high chemo-selectivity and activity of the Ni SAs catalyst,arising from the unique role of the single Ni-N3 site on simultaneously activating the H donor(N_(2)H_(4))and substrate,as well as the hydrogenation of the–NOH group as the rate-determining step.

关键词： single-atom catalyst chemo-selective reduction nitro compounds aromatic amines

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