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Construction of isolated Ni sites on nitrogen-doped hollow carbon spheres with Ni–N3 configuration for enhanced reduction of nitroarenes

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Abstract

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 mechanism. In 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 template. The 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 conditions. This TOF value is considerably superior to the supported Ni nanoparticle catalysts. The 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/NHCS. Density 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 (N2H4) and substrate, as well as the hydrogenation of the–NOH group as the rate-determining step.

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Acknowledgements

We acknowledge the financial assistance rendered by the National Natural Science Foundation of China (Nos. 21576243 and 21701168), Natural Science Foundation of Zhejiang Province (Nos. LY18B060006, LY17B060001, and LY21B030003), National Key R&D Program of China (No. 2020YFA0406101), Dalian high level talent innovation project (No. 2019RQ063), and Open project Foundation of State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (No. 20200021). We are also thankful to BL14W1 beamline of Shanghai Synchrotron Radiation Facility (SSRF) Shanghai for providing the beam time.

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  1. Binbin Feng, Rou Guo, and Qiulan Cai contributed equally to this work.

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  1. Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua, 321004, China

    Binbin Feng, Rou Guo, Qiulan Cai, Yaping Song, Nan Li, Yanghe Fu, De-Li Chen, Weidong Zhu & Fumin Zhang

  2. Dalian National Laboratory for Clean Energy & State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China

    Jiangwei Zhang

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  1. Binbin Feng
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Correspondence to De-Li Chen, Jiangwei Zhang, Weidong Zhu or Fumin Zhang.

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Construction of isolated Ni sites on nitrogen-doped hollow carbon spheres with Ni–N3 configuration for enhanced reduction of nitroarenes

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Feng, B., Guo, R., Cai, Q. et al. Construction of isolated Ni sites on nitrogen-doped hollow carbon spheres with Ni–N3 configuration for enhanced reduction of nitroarenes. Nano Res. 15, 6001–6009 (2022). https://doi.org/10.1007/s12274-022-4290-x

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