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A stable low-temperature H2-production catalyst by crowding Pt on α-MoC

Nature volume 589, pages 396–401 (2021)Cite this article

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Abstract

The water–gas shift (WGS) reaction is an industrially important source of pure hydrogen (H2) at the expense of carbon monoxide and water1,2. This reaction is of interest for fuel-cell applications, but requires WGS catalysts that are durable and highly active at low temperatures3. Here we demonstrate that the structure (Pt1–Ptn)/α-MoC, where isolated platinum atoms (Pt1) and subnanometre platinum clusters (Ptn) are stabilized on α-molybdenum carbide (α-MoC), catalyses the WGS reaction even at 313 kelvin, with a hydrogen-production pathway involving direct carbon monoxide dissociation identified. We find that it is critical to crowd the α-MoC surface with Pt1 and Ptn species, which prevents oxidation of the support that would cause catalyst deactivation, as seen with gold/α-MoC (ref. 4), and gives our system high stability and a high metal-normalized turnover number of 4,300,000 moles of hydrogen per mole of platinum. We anticipate that the strategy demonstrated here will be pivotal for the design of highly active and stable catalysts for effective activation of important molecules such as water and carbon monoxide for energy production.

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Fig. 1: Structural characterization and WGS performance of the Pt/α-MoC catalysts.
Fig. 2: WGS performance of the Pt/α-MoC catalysts and the typical WGS catalysts.
Fig. 3: Reaction route study.
Fig. 4: Stability of the Pt/α-MoC catalysts for the WGS reaction.

Data availability

The main data supporting the findings of this study are available within the paper and its Supplementary Information. Additional data are available from the corresponding authors upon reasonable request.

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Acknowledgements

This work received financial support from the Natural Science Foundation of China (21725301, 21932002, 21821004, 91645115, 51622211, 21577013, 21707015, 21872014, 21902018), the National Key R&D Program of China (2017YFB0602200, 2017YFA0700103, 2018YFA0305800), and the Beijing Outstanding Young Scientist Program (BJJWZYJH01201914430039). The X-ray absorption spectroscopy and X-ray diffraction experiments were conducted at the Shanghai Synchrotron Radiation Facility and the Beijing Synchrotron Radiation Facility. The Pt L3 edge X-ray absorption spectroscopy for 0.02 wt% Pt/α-MoC was conducted at beamline10-BM, MRCAT operations, Advanced Photon Source under contract number DEAC02-06CH11357. The AP-XPS experiments were conducted in Swiss Light Source synchrotron. D.M. acknowledges support from the Tencent Foundation through the XPLORER PRIZE.

Author information

Author notes

  1. These authors contributed equally: Xiao Zhang, Mengtao Zhang, Yuchen Deng, Mingquan Xu

Authors and Affiliations

  1. Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering and College of Engineering, and BIC-ESAT, Peking University, Beijing, China

    Xiao Zhang, Mengtao Zhang, Yuchen Deng, Xiaochen Zhang, Mi Peng, Jie Yan, Jinglin Xie & Ding Ma

  2. State Key Laboratory of Fine Chemicals, College of Chemical Engineering, Dalian University of Technology, Dalian, China

    Xiao Zhang, Bingbing Chen, Mingshu Bi & Chuan Shi

  3. School of Physical Sciences and CAS Key Laboratory of Vacuum Physics, University of Chinese Academy of Sciences, Beijing, China

    Mingquan Xu, Aowen Li, Jinan Shi & Wu Zhou

  4. Paul Scherrer Institute, Villigen, Switzerland

    Luca Artiglia & Jeroen A. van Bokhoven

  5. Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, China

    Wen Wen, Zheng Jiang & Xingyu Gao

  6. Shanghai Synchrotron Radiation Facility, Zhangjiang Lab, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, China

    Wen Wen, Zheng Jiang & Xingyu Gao

  7. Beijing Advanced Innovation Center for Materials Genome Engineering, Beijing, China

    Rui Gao, Yong-Wang Li & Xiaodong Wen

  8. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, China

    Rui Gao, Yong-Wang Li & Xiaodong Wen

  9. School of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, China

    Rui Gao

  10. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, China

    Siyu Yao

  11. Department of Chemical and Biological Engineering, Tufts University, Medford, MA, USA

    Sufeng Cao & Maria Flytzani-Stephanopoulos

  12. Chemical Science and Engineering Division, Argonne National Laboratory, Lemont, IL, USA

    Ce Yang & A. Jeremy Kropf

  13. Centre for Applied Research, NOVA Chemicals Corporation, Calgary, Alberta, Canada

    Ce Yang

  14. Institute of Chemical and Bioengineering, ETH Zurich, Zurich, Switzerland

    Jeroen A. van Bokhoven

  15. CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing, China

    Wu Zhou

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Contributions

D.M. conceived the project. D.M., W.Z., M.F.-S. and C.S. supervised the study. Xiao Zhang and M.Z. performed most of the reactions. M.X., A.L., J.S. and W.Z. performed the electron microscopy study. M.Z., Xiaochen Zhang, L.A. and J.A.v.B. did the NAP-XPS experiments. M.Z., J.Y. and B.C. did the TKA experiments. Y.D., M.P., C.Y., W.W., X.G., Z.J., S.Y. and A.J.K. performed the X-ray structure characterization (XAS and XRD) and analysis. S.Y. contributed to the calculation of the cost targets profile of the Au- or Pt-based WGS catalysts. M.Z., M.B. and J.X. did the XPS experiments. R.G., X.W. and Y.-W.L. did the DFT calculations. S.C. did the low-temperature reaction evaluation experiments. Xiao Zhang, M.Z., Y.D., W.Z., M.F.-S. and D.M. wrote the paper. All the authors discussed and revised the paper.

Corresponding authors

Correspondence to Chuan Shi, Wu Zhou or Ding Ma.

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The authors declare no competing interests.

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Peer review information Nature thanks Matteo Cargnello and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

This file contains Supplementary Figures S1-S19 and Supplementary Tables S1 and S2.

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Zhang, X., Zhang, M., Deng, Y. et al. A stable low-temperature H2-production catalyst by crowding Pt on α-MoC. Nature 589, 396–401 (2021). https://doi.org/10.1038/s41586-020-03130-6

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