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Achieving maximum overall light enhancement in plasmonic catalysis by combining thermal and non-thermal effects

Nature Catalysis volume 6, pages 1241–1247 (2023)Cite this article

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Abstract

Plasmonic photocatalysis presents a promising method for light-to-matter conversion. However, most current studies focus on understanding the relative importance of thermal and non-thermal effects while their synergistic effects remained less studied. Here we propose an index, termed overall light effectiveness, to capture the combined impact of these light effects on reactions. By systematic variation of the thickness of catalyst layers, we isolated both thermal and non-thermal contributions and optimized them to achieve maximum light enhancement. We demonstrate the approach using a carbon dioxide hydrogenation reaction on titania-supported rhodium nanoparticles as a model reaction system. It shows a generalizable potential in the design of catalyst systems with optimum combinations of heating and light illumination, especially with broadband light illumination such as sunlight, for achieving the most economical light-to-matter conversion in plasmonic catalysis.

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Fig. 1: Reactor set-up and calculated OLE.
Fig. 2: Separation of thermal and non-thermal contributions.
Fig. 3: Contributions from non-thermal and photothermal effects to total OLE.
Fig. 4: OLE under broadband white light illumination.

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Data availability

The data that support the findings of this paper are included in this manuscript and the Source Data. Data are also available from the corresponding author upon reasonable request. Source Data are provided with this paper.

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Acknowledgements

This work was supported by a grant from the National Science Foundation (no. CHE-1954838); the fund was used to support graduate students (Z.G. and Y.Y.) and access chemical supplies. Some characterizations were performed at the Duke University Shared Materials Instrumentation Facility, a member of the North Carolina Research Triangle Nanotechnology Network, which is supported by the National Science Foundation (award no. ECCS-2025064) as part of the National Nanotechnology Coordinated Infrastructure. We also thank H. O. Everitt from Army Research Laboratory-South for insightful discussions on this topic in general.

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  1. These authors contributed equally: Zhijia Geng, Yifan Yu.

Authors and Affiliations

  1. Department of Chemistry, Duke University, Durham, NC, USA

    Zhijia Geng, Yifan Yu, Abraham Joey Offen & Jie Liu

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  1. Zhijia Geng
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Contributions

J.L. conceived and supervised the research project. Z.G. and Y.Y. designed the experiments and carried out photocatalytic tests. Y.Y. fabricated photocatalysts and carried out SEM and X-ray photo-electron spectrometry characterization. Z.G. performed TEM characterization. A.J.O. contributed to the conceptual discussion and performed some of the initial experiments. Z.G. and Y.Y. analysed the results and wrote and revised the paper with input from the other authors.

Corresponding author

Correspondence to Jie Liu.

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Nature Catalysis thanks Vivek Polshettiwar and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Geng, Z., Yu, Y., Offen, A.J. et al. Achieving maximum overall light enhancement in plasmonic catalysis by combining thermal and non-thermal effects. Nat Catal 6, 1241–1247 (2023). https://doi.org/10.1038/s41929-023-01045-9

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