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Nano Research 2022, 15(12): 10006-10013 https://doi.org/10.1007/s12274-022-4294-6
Research Article | Issue | Published: 20 April 2022

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

Show Author's Information Yuemin Lin1,  Renfeng Nie4,  Yuting Li2,  Xun Wu3,  Jiaqi Yu3,  Shaohua Xie5,  Yajing Shen1,7,  Shanjun Mao6,  Yuzhuo Chen6,  Dan Lu1,  Zongbi Bao1,7,  Qiwei Yang1,7,  Qilong Ren1,7,  Yiwen Yang1,7,  Fudong Liu5,  Long Qi2( ),  Wenyu Huang3( ),  Zhiguo Zhang1,7( )
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, 38 Zheda Road, Hangzhou 310027, China
U.S. DOE Ames Laboratory, Iowa State University, Ames, Iowa 50011, USA
Department of Chemistry, Iowa State University, Ames, Iowa 50011, USA
College of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China
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
Advanced Materials and Catalysis Group, Institute of Catalysis, Department of Chemistry, Zhejiang University, Hangzhou 310028, China
Institute of Zhejiang University-Quzhou, Quzhou 324000, China
Keywords:
selective hydrogenation, 3-nitrostyrene, nitroarenes, cobalt single-atom, poisoning resistance
Topics:
Selective catalytic reduction
Cite this article:
Lin Y, Nie R, Li Y, et al. Highly efficient and anti-poisoning single-atom cobalt catalyst for selective hydrogenation of nitroarenes. Nano Research, 2022, 15(12): 10006-10013. https://doi.org/10.1007/s12274-022-4294-6
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Abstract Full text Electronic supplementary material About this article

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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Electronic supplementary material
About this article

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

Show Author's information Yuemin Lin1, Renfeng Nie4, Yuting Li2, Xun Wu3, Jiaqi Yu3, Shaohua Xie5, Yajing Shen1,7, Shanjun Mao6, Yuzhuo Chen6, Dan Lu1, Zongbi Bao1,7, Qiwei Yang1,7, Qilong Ren1,7, Yiwen Yang1,7, Fudong Liu5, Long Qi2( ), Wenyu Huang3( ), Zhiguo Zhang1,7( )
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, 38 Zheda Road, Hangzhou 310027, China
U.S. DOE Ames Laboratory, Iowa State University, Ames, Iowa 50011, USA
Department of Chemistry, Iowa State University, Ames, Iowa 50011, USA
College of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China
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
Advanced Materials and Catalysis Group, Institute of Catalysis, Department of Chemistry, Zhejiang University, Hangzhou 310028, China
Institute of Zhejiang University-Quzhou, Quzhou 324000, China

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.

Keywords: selective hydrogenation, 3-nitrostyrene, nitroarenes, cobalt single-atom, poisoning resistance

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Publication history
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Acknowledgements

Publication history

Received: 09 December 2021
Revised: 05 March 2022
Accepted: 06 March 2022
Published: 20 April 2022
Issue date: December 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

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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