Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions

Gonzalez-Carrero, Soranyel; Kosco, Jan; Fei, Teng; McCulloch, Iain; Durrant, James

doi:10.1039/d4sc04030a

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Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions

Soranyel Gonzalez-Carrero

, Jan Kosco, Teng Fei, Iain McCulloch

, James Durrant

Chemical Science

Swansea University Author: James Durrant

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DOI (Published version): 10.1039/d4sc04030a

Abstract

Organic heterojunction nanoparticles (NP) have recently gained significant interest as photocatalysts for visible light-driven hydrogen production. Whilst promising photocatalytic efficiencies have been reported for aqueous NP dispersions, the underlying dynamics of photogenerated charges in such or...

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Published in:	Chemical Science
ISSN:	2041-6520 2041-6539
Published:	Royal Society of Chemistry 2024
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URI:	https://cronfa.swan.ac.uk/Record/cronfa68082
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In contrast, on the slower μs to ms time range, the decay kinetics of heterojunction NP dispersion exhibited up to 15-fold larger amplitude and more than one order of magnitude slower decay of the photogenerated charges than those in films. The analysis of the nanomorphology, NP surfactant, polymer residual metal content and local polar environment suggest that the longer lifetime differences (in ms) in the charge recombination in NP dispersion are mostly associated with a charge carrier stabilisation on a shallow density of states on the NP surface of ∼350 meV by interaction with local water environment, resulting in suppressed charge recombination. 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spelling	v2 68082 2024-10-28 Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions f3dd64bc260e5c07adfa916c27dbd58a 0000-0001-8353-7345 James Durrant James Durrant true false 2024-10-28 EAAS Organic heterojunction nanoparticles (NP) have recently gained significant interest as photocatalysts for visible light-driven hydrogen production. Whilst promising photocatalytic efficiencies have been reported for aqueous NP dispersions, the underlying dynamics of photogenerated charges in such organic heterojunction photocatalysts and how these might differ from more widely studied dry heterojunction films remain relatively unexplored. In this study, we combine transient optical spectroscopies over twelve orders of magnitude in time, using pulsed and continuous light illumination, to elucidate the differences in the charge carrier dynamics of heterojunction NP dispersions, dried NP films, and bulk heterojunction films prepared by spin coating. The ultrafast fast (ps to ns) transient absorption results show efficient charge generation and indistinguishable nanosecond charge recombination decay kinetics of separated charges in all three samples. In contrast, on the slower μs to ms time range, the decay kinetics of heterojunction NP dispersion exhibited up to 15-fold larger amplitude and more than one order of magnitude slower decay of the photogenerated charges than those in films. The analysis of the nanomorphology, NP surfactant, polymer residual metal content and local polar environment suggest that the longer lifetime differences (in ms) in the charge recombination in NP dispersion are mostly associated with a charge carrier stabilisation on a shallow density of states on the NP surface of ∼350 meV by interaction with local water environment, resulting in suppressed charge recombination. The lengthening of NP dispersion charge carrier lifetime is discussed regarding the energetic loss for function and their implications in photocatalysis. Journal Article Chemical Science Royal Society of Chemistry 2041-6520 2041-6539 21 10 2024 2024-10-21 10.1039/d4sc04030a COLLEGE NANME Engineering and Applied Sciences School COLLEGE CODE EAAS Swansea University Not Required We acknowledge financial support from the EPSRC project ATIP (EP/TO28513/1), KAUST (OSR-2018-CRG7-3749.2), from the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement no. 886664, and Generalitat de Valencia (CIDEIG/2023/17) (S. G.-C.). IM acknowledges financial support from KAUST Office of Sponsored Research CRG10, by EU Horizon2020 grant agreement no. 952911, BOOSTER, grant agreement no. 862474, RoLA-FLEX, and grant agreement no. 101007084 CITYSOLAR, as well as EPSRC Projects EP/T026219/1, EP/W017091/1, and EP/L011972/1. 2024-10-28T15:10:43.8769190 2024-10-28T14:53:05.0249619 Faculty of Science and Engineering School of Engineering and Applied Sciences - Materials Science and Engineering Soranyel Gonzalez-Carrero 0000-0003-2430-4458 1 Jan Kosco 2 Teng Fei 3 Iain McCulloch 0000-0002-6340-7217 4 James Durrant 0000-0001-8353-7345 5 68082__32754__c31fd58e346c437f8f6e120cf0f81c7e.pdf 68082.VOR.pdf 2024-10-28T14:59:45.1707824 Output 1854276 application/pdf Version of Record true © 2024 The Author(s). This Open Access Article is licensed under a Creative Commons Attribution 3.0 Unported Licence (CC BY 3.0). true eng http://creativecommons.org/licenses/by/3.0/
title	Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions
spellingShingle	Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions James Durrant
title_short	Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions
title_full	Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions
title_fullStr	Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions
title_full_unstemmed	Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions
title_sort	Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions
author_id_str_mv	f3dd64bc260e5c07adfa916c27dbd58a
author_id_fullname_str_mv	f3dd64bc260e5c07adfa916c27dbd58a_***_James Durrant
author	James Durrant
author2	Soranyel Gonzalez-Carrero Jan Kosco Teng Fei Iain McCulloch James Durrant
format	Journal article
container_title	Chemical Science
publishDate	2024
institution	Swansea University
issn	2041-6520 2041-6539
doi_str_mv	10.1039/d4sc04030a
publisher	Royal Society of Chemistry
college_str	Faculty of Science and Engineering
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hierarchy_top_title	Faculty of Science and Engineering
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hierarchy_parent_title	Faculty of Science and Engineering
department_str	School of Engineering and Applied Sciences - Materials Science and Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Materials Science and Engineering
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description	Organic heterojunction nanoparticles (NP) have recently gained significant interest as photocatalysts for visible light-driven hydrogen production. Whilst promising photocatalytic efficiencies have been reported for aqueous NP dispersions, the underlying dynamics of photogenerated charges in such organic heterojunction photocatalysts and how these might differ from more widely studied dry heterojunction films remain relatively unexplored. In this study, we combine transient optical spectroscopies over twelve orders of magnitude in time, using pulsed and continuous light illumination, to elucidate the differences in the charge carrier dynamics of heterojunction NP dispersions, dried NP films, and bulk heterojunction films prepared by spin coating. The ultrafast fast (ps to ns) transient absorption results show efficient charge generation and indistinguishable nanosecond charge recombination decay kinetics of separated charges in all three samples. In contrast, on the slower μs to ms time range, the decay kinetics of heterojunction NP dispersion exhibited up to 15-fold larger amplitude and more than one order of magnitude slower decay of the photogenerated charges than those in films. The analysis of the nanomorphology, NP surfactant, polymer residual metal content and local polar environment suggest that the longer lifetime differences (in ms) in the charge recombination in NP dispersion are mostly associated with a charge carrier stabilisation on a shallow density of states on the NP surface of ∼350 meV by interaction with local water environment, resulting in suppressed charge recombination. The lengthening of NP dispersion charge carrier lifetime is discussed regarding the energetic loss for function and their implications in photocatalysis.
published_date	2024-10-21T15:10:42Z
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score	11.036203

Impact of water solvation on the charge carrier dynamics of organic heterojunction photocatalyst nanoparticle dispersions

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