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Nano Research 2023, 16(2): 2302-2310 https://doi.org/10.1007/s12274-022-5277-3
Research Article | Issue | Published: 27 October 2022

Determining the contribution of Mo single atoms components in MoO2 nanocatalyst in transfer hydrogenation

Show Author's Information Ze-Nan Hu1,2,  Yongjian Ai3,  Yan Zhao4,  Yiming Wang2,  Kelong Ding2,  Wenhui Zhang2,  Rongxiu Guo2,  Xinyue Zhang2,  Xiangbin Cai5,  Ning Wang5,  Jianshe Hu2,  Qionglin Liang3,  Hongyang Liu6,  Fei Huang6( ),  Limin Wu4,  Jiangwei Zhang4( ),  Hong-bin Sun2( )
School of Environmental Engineering and Chemistry, Luoyang Institute of Science and Technology, Luoyang 471023, China
Department of Chemistry, Northeastern University, Shenyang 110819, China
MOE Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology, Beijing Key Lab of Microanalytical Methods & Instrumentation, Department of Chemistry, Center for Synthetic and Systems Biology, Tsinghua University, Beijing 100084, China
College of Energy Material and Chemistry, Inner Mongolia University, Hohhot 010021, China
Department of Physics and Center for Quantum Materials, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong SAR, China
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
Keywords:
synergistic effect, transfer hydrogenation, nitroarenes, Mo single atoms, MoO2 nanocatalyst
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Hu Z-N, Ai Y, Zhao Y, et al. Determining the contribution of Mo single atoms components in MoO2 nanocatalyst in transfer hydrogenation. Nano Research, 2023, 16(2): 2302-2310. https://doi.org/10.1007/s12274-022-5277-3
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Abstract Full text Electronic supplementary material About this article

Nanocatalysts are likely to contain undetected single-atom components, which may have been ignored but have significant effect in catalytic reactions. Herein, we report a catalyst composed of Mo single atoms (SAs) and MoO2 nanoparticles (NPs) (MoSAs-MoO2@NC), which is an exact model to understand how the SAs contribute to the nanocatalyst. Both experimental results and the density functional theory calculations reveal that Mo SAs on nitrogen-doped carbon provides the reaction zone for nitro reduction, while MoO2 is the active site for decomposing hydrazine hydrate to produce H*. Thanks to the synergy between Mo SAs and MoO2 NPs, this catalyst exhibits noble metal-like catalytic activity (100% conversion at 4 min) for the dechlorination-proof transfer hydrogenation. Additionally, the hydrogen migration on the catalyst is verified by the electrochemical tests in the absence of a hydrogen source. This work provides a model for further study on the coexistence of single atoms in nanoparticle catalysts.


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About this article

Determining the contribution of Mo single atoms components in MoO2 nanocatalyst in transfer hydrogenation

Show Author's information Ze-Nan Hu1,2, Yongjian Ai3, Yan Zhao4, Yiming Wang2, Kelong Ding2, Wenhui Zhang2, Rongxiu Guo2, Xinyue Zhang2, Xiangbin Cai5, Ning Wang5, Jianshe Hu2, Qionglin Liang3, Hongyang Liu6, Fei Huang6( ), Limin Wu4, Jiangwei Zhang4( ), Hong-bin Sun2( )
School of Environmental Engineering and Chemistry, Luoyang Institute of Science and Technology, Luoyang 471023, China
Department of Chemistry, Northeastern University, Shenyang 110819, China
MOE Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology, Beijing Key Lab of Microanalytical Methods & Instrumentation, Department of Chemistry, Center for Synthetic and Systems Biology, Tsinghua University, Beijing 100084, China
College of Energy Material and Chemistry, Inner Mongolia University, Hohhot 010021, China
Department of Physics and Center for Quantum Materials, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong SAR, China
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China

Abstract

Nanocatalysts are likely to contain undetected single-atom components, which may have been ignored but have significant effect in catalytic reactions. Herein, we report a catalyst composed of Mo single atoms (SAs) and MoO2 nanoparticles (NPs) (MoSAs-MoO2@NC), which is an exact model to understand how the SAs contribute to the nanocatalyst. Both experimental results and the density functional theory calculations reveal that Mo SAs on nitrogen-doped carbon provides the reaction zone for nitro reduction, while MoO2 is the active site for decomposing hydrazine hydrate to produce H*. Thanks to the synergy between Mo SAs and MoO2 NPs, this catalyst exhibits noble metal-like catalytic activity (100% conversion at 4 min) for the dechlorination-proof transfer hydrogenation. Additionally, the hydrogen migration on the catalyst is verified by the electrochemical tests in the absence of a hydrogen source. This work provides a model for further study on the coexistence of single atoms in nanoparticle catalysts.

Keywords: synergistic effect, transfer hydrogenation, nitroarenes, Mo single atoms, MoO2 nanocatalyst

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Acknowledgements

Publication history

Received: 27 October 2022
Accepted: 28 October 2022
Published: 27 October 2022
Issue date: February 2023

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was financially supported by the National Key R&D Program of China (Nos. 2021YFA1502802 and 2020YFA0406101), the National Natural Science Foundation of China (Nos. 21961160722, 21872020, 22072162, 91845201, and 21701168), the Liaoning Revitalization Talents Program XLYC1907055, Natural Science Foundation of Liaoning Province (No. 2021-MS-001), Dalian National Lab for Clean Energy (DNL Cooperation Fund 202001), and Dalian high level talent innovation project (No. 2019RQ063). We gratefully acknowledge 07A1 beamline of Taiwan Light Source (TLS) of the “National Synchrotron Radiation Research Center” (NSRRC), China for providing the beam time.

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