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Highly efficient and anti-poisoning single-atom cobalt catalyst for selective hydrogenation of nitroarenes

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Abstract

Developing non-precious metal catalysts to selectively reduce functionalized nitroarenes with high efficiency is urgently desirable for the production of value-added amines. Herein, we report a novel, efficient, anti-poisoning single-atom cobalt catalyst (Co-NAC) for the highly selective hydrogenation of the nitro to amino group for nitroarenes baring various functional groups, including vinyl, cyano, and halogen. Using a combination of structure characterization techniques, we have confirmed that the cobalt species are predominantly present in the form of four-coordinated Co single sites anchored on nitrogen-assembly carbon (NAC) as the ordered mesoporous support. Co-NAC catalysts enable the full conversion and > 99% selectivity with molecular H2 as a green reductant under mild conditions (80 °C, 2 MPa H2). As for the selective hydrogenation of 3-nitrostyrene, Co-NAC catalyst affords high catalytic productivity (19.7 h−1), which is superior to the cobalt nanoparticles (NPs) catalysts and most of the recently reported Co-based catalysts. This is attributed to the highly accessible atomically-dispersed Co active sites, the high surface area with ordered-mesoporous morphology and the prominent high content of nitrogen dopants. Notably, Co-NAC catalyst displays resistance towards sulfur-containing poisons (20 equivalents) and strong non-oxidizing acid (8 M), showing great potential for continuous application in the chemical industry.

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Acknowledgements

This work was supported by the National Key R&D Program of China (No. 2016YFA0202900), and the National Natural Science Foundation of China (Nos. 21878266, 22078288, and 22108243). L. Q. and Y. T. L. were supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. The Ames Laboratory is operated for the U.S. DOE by Iowa State University under Contract No. DE-AC02-07CH11358. W. Y. H., J. Q. Y., and X. W. thank the support from Iowa State University. F. D. L. thanks the Startup Fund from the University of Central Florida (UCF). S. H. X. thanks the support from the Preeminent Postdoctoral Program (P3) at UCF. This research used beamline 7-BM (QAS) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704.

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Authors and Affiliations

  1. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, 38 Zheda Road, Hangzhou, 310027, China

    Yuemin Lin, Yajing Shen, Dan Lu, Zongbi Bao, Qiwei Yang, Qilong Ren, Yiwen Yang & Zhiguo Zhang

  2. U.S. DOE Ames Laboratory, Iowa State University, Ames, Iowa, 50011, USA

    Yuting Li & Long Qi

  3. Department of Chemistry, Iowa State University, Ames, Iowa, 50011, USA

    Xun Wu, Jiaqi Yu & Wenyu Huang

  4. College of Chemical Engineering, Zhengzhou University, Zhengzhou, 450001, China

    Renfeng Nie

  5. Department of Civil, Environmental, and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC), University of Central Florida, Orlando, FL, 32816, USA

    Shaohua Xie & Fudong Liu

  6. Advanced Materials and Catalysis Group, Institute of Catalysis, Department of Chemistry, Zhejiang University, Hangzhou, 310028, China

    Shanjun Mao & Yuzhuo Chen

  7. Institute of Zhejiang University-Quzhou, Quzhou, 324000, China

    Yajing Shen, Zongbi Bao, Qiwei Yang, Qilong Ren, Yiwen Yang & Zhiguo Zhang

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  1. Yuemin Lin
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Correspondence to Long Qi, Wenyu Huang or Zhiguo Zhang.

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Lin, Y., Nie, R., Li, Y. et al. Highly efficient and anti-poisoning single-atom cobalt catalyst for selective hydrogenation of nitroarenes. Nano Res. 15, 10006–10013 (2022). https://doi.org/10.1007/s12274-022-4294-6

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