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Research Article

Tuning the coordination environment of single-atom catalyst M-N-C towards selective hydrogenation of functionalized nitroarenes

Dan Zhou1,2, Leilei Zhang2( ), Xiaoyan Liu2, Haifeng Qi2, Qinggang Liu2, Ji Yang2, Yang Su2, Jingyuan Ma3, Jianzhong Yin2( ), Aiqin Wang2( )
School of Chemical Engineering State Key Laboratory of Fine Chemicals Dalian University of Technology Dalian 116024 China
CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China
Shanghai Synchrotron Radiation Facility Zhangjiang Laboratory (SSRF, ZJLab) Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China
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An erratum to this article is available online at:
https://doi.org/10.1007/s12274-021-3739-7

Graphical Abstract

Abstract

Fine-tuning of the coordination environment of single-atom catalysts (SACs) is effective to optimize their catalytic performances, yet it remains challenging due to the vulnerability of SACs. Herein, we report a new approach to engineering the coordination environment of M-N-C (M = Fe, Co, and Ni) SACs by using glutamic acid as the N/C source and pyrolysis atmosphere as a regulator. Compared with that in N2, NH3 was able to promote the doping of N at T < 700 ℃ yet etch the N-species at higher temperatures, by which the M-N coordination number (CN) and the electronic structure were delicately tuned. It was found that the electron density of Ni single atoms increased with the decrease of Ni-N CN. As a consequence, the capability of Ni-N-C to dissociate H2 was greatly enhanced and a higher catalytic activity in chemoselective hydrogenation of functionalized nitroarenes was achieved. Moreover, this modulation method could be applied to other transition metals including Fe and Co. In particular, the as-synthesized Co-N-C SAC afforded a turnover frequency of 152.3 h−1 with 99% selectivity to 3-vinylaniline in the hydrogenation of 3-nitrostyrene, which was the highest ever reported thus far and was at least one order of magnitude more active than state-of-the-art noble-metal-free M-N-C catalysts, demonstrating the great potential of engineering the coordination environment of SACs.

Keywords

single-atom catalystscoordination environmentNi-N-Cchemoselective hydrogenationpyrolysis atmosphere

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Nano Research
Volume 15 Issue 1,
January 2022
Pages 519-527
DOI: 10.1007/s12274-021-3511-z
Cite this article:
Zhou D, Zhang L, Liu X, et al. Tuning the coordination environment of single-atom catalyst M-N-C towards selective hydrogenation of functionalized nitroarenes. Nano Research, 2022, 15(1): 519-527. https://doi.org/10.1007/s12274-021-3511-z
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Received: 01 March 2021
Revised: 06 April 2021
Accepted: 08 April 2021
Published: 11 June 2021
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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