Defect-driven nanostructuring of low-nuclearity Pt-Mo ensembles for continuous gas-phase formic acid dehydrogenation

Luyao Guo, Kaixuan Zhuge, Siyang Yan, Shiyi Wang, Jia Zhao (), Saisai Wang, Panzhe Qiao, Jiaxu Liu (), Xiaoling Mou, Hejun Zhu (), Ziang Zhao, Li Yan, Ronghe Lin () and Yunjie Ding ()
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Luyao Guo: Zhejiang Normal University
Kaixuan Zhuge: Zhejiang University of Technology
Siyang Yan: Dalian University of Technology
Shiyi Wang: Zhejiang Normal University
Jia Zhao: Zhejiang University of Technology
Saisai Wang: Zhejiang University of Technology
Panzhe Qiao: Chinese Academy of Sciences
Jiaxu Liu: Dalian University of Technology
Xiaoling Mou: Zhejiang Normal University
Hejun Zhu: Chinese Academy of Sciences
Ziang Zhao: Chinese Academy of Sciences
Li Yan: Chinese Academy of Sciences
Ronghe Lin: Zhejiang Normal University
Yunjie Ding: Zhejiang Normal University

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract Supported metal clusters comprising of well-tailored low-nuclearity heteroatoms have great potentials in catalysis owing to the maximized exposure of active sites and metal synergy. However, atomically precise design of these architectures is still challenging for the lack of practical approaches. Here, we report a defect-driven nanostructuring strategy through combining defect engineering of nitrogen-doped carbons and sequential metal depositions to prepare a series of Pt and Mo ensembles ranging from single atoms to sub-nanoclusters. When applied in continuous gas-phase decomposition of formic acid, the low-nuclearity ensembles with unique Pt3Mo1N3 configuration deliver high-purity hydrogen at full conversion with unexpected high activity of 0.62 molHCOOH molPt−1 s−1 and remarkable stability, significantly outperforming the previously reported catalysts. The remarkable performance is rationalized by a joint operando dual-beam Fourier transformed infrared spectroscopy and density functional theory modeling study, pointing to the Pt-Mo synergy in creating a new reaction path for consecutive HCOOH dissociations.

Date: 2023
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DOI: 10.1038/s41467-023-42759-5

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