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Steam methane reforming using a regenerable antenna–reactor plasmonic photocatalyst

Nature Catalysis volume 7, pages 1339–1349 (2024)Cite this article

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Abstract

Steam methane reforming (SMR) is the major industrial process for hydrogen production. It currently relies on high-temperature operating conditions and is associated with high carbon intensity. Photocatalytic SMR could provide greener and potentially more efficient H2 production. Here we demonstrate a plasmonic photocatalytic approach based on a Cu–Rh antenna–reactor photocatalyst for highly reactive, selective and stable SMR due to plasmon-mediated hot carrier contributions. We observe that the photocatalyst is intrinsically stable in photocatalysis but deactivates under thermocatalysis; however, the thermally deactivated catalyst can be regenerated by resonant illumination. The regeneration mechanism is studied in detail and found to be caused by plasmon-induced associative desorption of oxygen and carbon species.

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Fig. 1: Photocatalytic SMR.
Fig. 2: Study of the mechanism of photocatalytic SMR.
Fig. 3: Thermocatalytic deactivation and photocatalytic regeneration.
Fig. 4: Study of the mechanism of photocatalytic regeneration.

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Data availability

Additional datasets generated and/or analysed during the current study that are not included in the published Article and associated Supplementary Information, including the atomic coordinates for the JDFTx calculations, are available from the open-access Zenodo repository at https://doi.org/10.5281/zenodo.13377300 (ref. 66).

Code availability

Python codes for the EM simulation and hot carrier distribution calculations are available from the open-access Zenodo repository at https://doi.org/10.5281/zenodo.13377300 (ref. 66).

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Acknowledgements

This article is based on work supported by the Robert A. Welch Foundation under grants C-1220 (to N.J.H.) and C-1222 (to P.N.) and by the Air Force Office of Scientific Research via the Department of Defense Multidisciplinary University Research Initiative under AFOSR Award number FA9550-15-1-0022. We acknowledge B. Chen from the Shared Equipment Authority at Rice University for providing valuable insights and assistance with processing the XPS data.

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Authors and Affiliations

  1. Department of Chemistry, Rice University, Houston, TX, USA

    Yigao Yuan, Aaron Bayles, Hossein Robatjazi & Naomi J. Halas

  2. Department of Materials Science and NanoEngineering, Rice University, Houston, TX, USA

    Jingyi Zhou & Peter Nordlander

  3. Syzygy Plasmonics, Houston, TX, USA

    Hossein Robatjazi

  4. Department of Electrical and Computer Engineering, Rice University, Houston, TX, USA

    Peter Nordlander & Naomi J. Halas

  5. Department of Physics and Astronomy, Rice University, Houston, TX, USA

    Peter Nordlander & Naomi J. Halas

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  1. Yigao Yuan
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Contributions

Y.Y., P.N. and N.J.H. initiated the project. Y.Y. developed the photocatalyst, performed the characterization, studied the catalysis and analysed the data. J.Z. performed the theoretical simulations. A.B. performed the scanning transmission electron microscopy. H.R. helped to interpret the data. P.N. and N.J.H. supervised the research. All authors contributed to preparation of the manuscript.

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Correspondence to Peter Nordlander or Naomi J. Halas.

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Competing interests

The antenna–reactor concept is protected under US patents US10766024B2 and US11958043B2, with additional coverage pending in published US patent application US20210023541A1. The antenna–reactor concept is also described in the international patent application WO 2018/231398 A2. Syzygy Plasmonics owns several patents relating to the photoreactor platform. N.J.H. and P.N. are co-founders of Syzygy Plasmonics. N.J.H., P.N. and H.R. have interest in Syzygy Plasmonics and hold equity in the company. The remaining authors declare no competing interests.

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Nature Catalysis thanks Jennifer Dionne, Hisao Yoshida and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Yuan, Y., Zhou, J., Bayles, A. et al. Steam methane reforming using a regenerable antenna–reactor plasmonic photocatalyst. Nat Catal 7, 1339–1349 (2024). https://doi.org/10.1038/s41929-024-01248-8

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