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Unassisted Highly Selective Gas-Phase CO₂ Reduction with a Plasmonic Au/p-GaN Photocatalyst Using H₂O as an Electron Donor

Li, Rengui and Cheng, Wen-Hui and Richter, Matthias H. and DuChene, Joseph S. and Tian, Wenming and Li, Can and Atwater, Harry A. (2021) Unassisted Highly Selective Gas-Phase CO₂ Reduction with a Plasmonic Au/p-GaN Photocatalyst Using H₂O as an Electron Donor. ACS Energy Letters, 6 (5). pp. 1849-1856. ISSN 2380-8195. doi:10.1021/acsenergylett.1c00392. https://resolver.caltech.edu/CaltechAUTHORS:20210423-164855164

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Abstract

Surface plasmon resonances in metal nanostructures enable the generation of nonequilibrium hot electron–hole pairs, which has received wide interest as a means to drive chemical reactions at the nanoscale. However, harvesting hot holes in plasmonic heterostructures to drive oxidation reactions to balance the photocatalytic CO₂ reduction reaction has been challenging. Further, details of the balanced redox reaction pathways for gas-phase photocatalysis have been difficult to identify. Here, we report an Au/p-GaN plasmonic heterostructure photocatalyst in which unassisted, self-sustaining, highly selective photocatalytic CO₂ reduction to CO is directly balanced by water oxidation, operating under solar illumination. We find remarkable enhancements in CO yield for heterostructures that employ a metal/insulator/semiconductor configuration with an ultrathin aluminum oxide layer between composite Au/Cu nanoparticles and p-GaN. Our work underscores the potential for plasmonic heterostructure photocatalysts to perform selective and unassisted gas-phase photocatalytic CO₂ reduction to convert solar energy into chemical fuels.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acsenergylett.1c00392DOIArticle
ORCID:
AuthorORCID
Li, Rengui0000-0002-8099-0934
Cheng, Wen-Hui0000-0003-3233-4606
Richter, Matthias H.0000-0003-0091-2045
DuChene, Joseph S.0000-0002-7145-323X
Li, Can0000-0002-9301-7850
Atwater, Harry A.0000-0001-9435-0201
Alternate Title:Unassisted Highly Selective Gas-Phase CO2 Reduction with a Plasmonic Au/p-GaN Photocatalyst Using H2O as an Electron Donor
Additional Information:© 2021 American Chemical Society. Received: February 21, 2021; Accepted: April 15, 2021; Published: April 20, 2021. This work was performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, and was primarily supported through the Office of Science of the U.S. Department of Energy (DOE) under Award No. DE SC0004993 (sample synthesis, gas-phase photocatalytic measurements, and photoelectrochemical measurements), and by the Liquid Sunlight Alliance under Award No. DESC0021266 (sample structural and morphological characterization and data analysis). Research was in part carried out at the Molecular Materials Research Center of the Beckman Institute of the California Institute of Technology. Author Contributions. R.L. and W.-H.C. contributed equally to this work. R.L., W.-H.C., and H.A.A. developed the ideas. R.L. and W.-H.C. fabricated the samples and performed the measurements, with assistance from M.H.R., J.S.D., and W.T. The manuscript was written by R.L., W.-H.C., J.S.D., and H.A.A., with input from all authors. All authors contributed to the discussion and interpretation of results as well as the presentation and preparation of the manuscript. The authors declare no competing financial interest.
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-SC0021266
Issue or Number:5
DOI:10.1021/acsenergylett.1c00392
Record Number:CaltechAUTHORS:20210423-164855164
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210423-164855164
Official Citation:Unassisted Highly Selective Gas-Phase CO2 Reduction with a Plasmonic Au/p-GaN Photocatalyst Using H2O as an Electron Donor. Rengui Li, Wen-Hui Cheng, Matthias H. Richter, Joseph S. DuChene, Wenming Tian, Can Li, and Harry A. Atwater. ACS Energy Letters 2021 6 (5), 1849-1856; DOI: 10.1021/acsenergylett.1c00392
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108829
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:28 Apr 2021 14:30
Last Modified:17 May 2021 18:05

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