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Proton-assisted electron transfer and hydrogen-atom diffusion in a model system for photocatalytic hydrogen production

Zhang, Yuanzheng and Dai, Yunrong and Li, Huihui and Yin, Lifeng and Hoffmann, Michael R. (2020) Proton-assisted electron transfer and hydrogen-atom diffusion in a model system for photocatalytic hydrogen production. Communications Materials, 1 . Art. No. 66. ISSN 2662-4443. PMCID PMC7505813. https://resolver.caltech.edu/CaltechAUTHORS:20200922-133041984

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Abstract

Solar energy can be converted into chemical energy by photocatalytic water splitting to produce molecular hydrogen. Details of the photo-induced reaction mechanism occurring on the surface of a semiconductor are not fully understood, however. Herein, we employ a model photocatalytic system consisting of single atoms deposited on quantum dots that are anchored on to a primary photocatalyst to explore fundamental aspects of photolytic hydrogen generation. Single platinum atoms (Pt₁) are anchored onto carbon nitride quantum dots (CNQDs), which are loaded onto graphitic carbon nitride nanosheets (CNS), forming a Pt₁@CNQDs/CNS composite. Pt₁@CNQDs/CNS provides a well-defined photocatalytic system in which the electron and proton transfer processes that lead to the formation of hydrogen gas can be investigated. Results suggest that hydrogen bonding between hydrophilic surface groups of the CNQDs and interfacial water molecules facilitates both proton-assisted electron transfer and sorption/desorption pathways. Surface bound hydrogen atoms appear to diffuse from CNQDs surface sites to the deposited Pt₁ catalytic sites leading to higher hydrogen-atom fugacity surrounding each isolated Pt₁ site. We identify a pathway that allows for hydrogen-atom recombination into molecular hydrogen and eventually to hydrogen bubble evolution.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1038/s43246-020-00068-0DOIArticle
https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7505813PubMed CentralArticle
ORCID:
AuthorORCID
Zhang, Yuanzheng0000-0002-7584-5695
Li, Huihui0000-0002-3823-1010
Yin, Lifeng0000-0002-5181-195X
Hoffmann, Michael R.0000-0001-6495-1946
Additional Information:© The Author(s) 2020. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. Received 27 January 2020; Accepted 02 July 2020; Published 21 September 2020. This work was financially supported by the National Natural Science Foundation of China (Grant 21777009), the Bill and Melinda Gates Foundation (BMGF RTTC Grants OPP1111246 and OPP1149755), Beijing Natural Science Foundation (Grant 8182031), and Major Science and Technology Program for Water Pollution Control and Treatment (Grant 2018ZX07109). Data availability: The authors declare that all the data supporting the findings of this study are available within the paper and its Supplementary Information. Author Contributions: Y.Z., Y.D., and H.L. prepared, characterized, and tested the catalysts. Y.D. performed the spectrum related experiments. Y.Z. and L.Y. collected and analyzed the data. Y.Z. and L.Y. wrote the paper in discussion with M.H. L.Y. and M.H. supervised the overall project. The authors declare no competing interests.
Funders:
Funding AgencyGrant Number
National Natural Science Foundation of China21777009
Bill and Melinda Gates FoundationOPP1111246
Bill and Melinda Gates FoundationOPP1149755
Beijing Municipal Natural Science Foundation8182031
Major Science and Technology Program for Water Pollution Control and Treatment2018ZX07109
PubMed Central ID:PMC7505813
Record Number:CaltechAUTHORS:20200922-133041984
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200922-133041984
Official Citation:Zhang, Y., Dai, Y., Li, H. et al. Proton-assisted electron transfer and hydrogen-atom diffusion in a model system for photocatalytic hydrogen production. Commun Mater 1, 66 (2020). https://doi.org/10.1038/s43246-020-00068-0
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:105474
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:22 Sep 2020 20:39
Last Modified:07 Oct 2020 16:25

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