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Research Article

Breaking the activity limitation of iridium single-atom catalyst in hydrogenation of quinoline with synergistic nanoparticles catalysis

Qikai Shen1,2, Hongqiang Jin1,2, Peipei Li1,2, Xiaohu Yu3, Lirong Zheng4, Weiguo Song1,2( ), Changyan Cao1,2( )
Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
University of Chinese Academy of Sciences, Beijing 100049, China
Institute of Theoretical and Computational Chemistry, Shaanxi Key Laboratory of Catalysis, School of Chemical & Environment Sciences, Shaanxi University of Technology, Hanzhong 723000, China
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
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Graphical Abstract

Synergistic iridium single atoms and nanoparticles catalyst exhibits unprecedentedly activity forquinoline hydrogenation.

Abstract

Single-atom catalysts (SACs) with the advantages of homogeneous and heterogeneous catalysts have become a hot-spot in catalysis field. However, for lack of metal–metal bond in SACs, H2 has to go through heterolytic dissociation pathway, which has higher barrier than homolytic dissociation pathway, and thus limits the hydrogenation activity of SACs. Herein, we propose and demonstrate through constructing synergistic iridium single atoms and nanoparticles co-existed catalyst (denoted as Ir1+NPs/CMK) to boost the catalytic activity of quinoline hydrogenation. Both experimental and density functional theory calculation results confirm that Ir1 single sites activate quinoline, while Ir nanoparticles boost hydrogen dissociation. H atoms generated at Ir nanoparticles migrate to the quinoline bounded Ir1 single sites to complete hydrogenation. The Ir1+NPs/CMK catalyst exhibits much higher reactivity with turnover frequency of 7,800 h−1 than those counterpart Ir1/CMK and IrNPs/CMK catalysts, and is 20,000 times higher activity of commercial Ir/C benchmark catalyst for hydrogenation of quinoline under the same reaction conditions. This synergistic catalysis strategy between single atoms and nanoparticles provides a solution to further improve the performance of SACs for hydrogenation.

Keywords

heterogeneous catalysissingle atomsynergisticquinolinehydrogenation

Electronic Supplementary Material

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Nano Research
Volume 15 Issue 6,
June 2022
Pages 5024-5031
DOI: 10.1007/s12274-022-4235-4
Cite this article:
Shen Q, Jin H, Li P, et al. Breaking the activity limitation of iridium single-atom catalyst in hydrogenation of quinoline with synergistic nanoparticles catalysis. Nano Research, 2022, 15(6): 5024-5031. https://doi.org/10.1007/s12274-022-4235-4
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Received: 20 January 2022
Revised: 11 February 2022
Accepted: 13 February 2022
Published: 22 March 2022
© Tsinghua University Press 2022
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