Generation of long-lived charges in organic semiconductor heterojunction nanoparticles for efficient photocatalytic hydrogen evolution

Jan Kosco; Soranyel Gonzalez-Carrero; Calvyn T. Howells; Teng Fei; Yifan Dong; Rachid Sougrat; George T. Harrison; Yuliar Firdaus; Rajendar Sheelamanthula; Balaji Purushothaman; Floriana Moruzzi; Weidong Xu; Lingyun Zhao; Aniruddha Basu; Stefaan De Wolf; Thomas D. Anthopoulos; James R. Durrant; Iain McCulloch

doi:10.1038/s41560-022-00990-2

Generation of long-lived charges in organic semiconductor heterojunction nanoparticles for efficient photocatalytic hydrogen evolution

Jan Kosco^*, Soranyel Gonzalez-Carrero, Calvyn T. Howells, Teng Fei, Yifan Dong, Rachid Sougrat, George T. Harrison, Yuliar Firdaus, Rajendar Sheelamanthula, Balaji Purushothaman, Floriana Moruzzi, Weidong Xu, Lingyun Zhao, Aniruddha Basu, Stefaan De Wolf, Thomas D. Anthopoulos, James R. Durrant^*, Iain McCulloch^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

224 Scopus citations

Abstract

Organic semiconductor photocatalysts for the production of solar fuels are attractive as they can be synthetically tuned to absorb visible light while simultaneously retaining suitable energy levels to drive a range of processes. However, a greater understanding of the photophysics that determines the function of organic semiconductor heterojunction nanoparticles is needed to optimize performance. Here, we show that such materials can intrinsically generate remarkably long-lived reactive charges, enabling them to efficiently drive sacrificial hydrogen evolution. Our optimized hetereojunction photocatalysts comprise the conjugated polymer PM6 matched with Y6 or PCBM electron acceptors, and achieve external quantum efficiencies of 1.0% to 5.0% at 400 to 900 nm and 8.7% to 2.6% at 400 to 700 nm, respectively. Employing transient and operando spectroscopies, we find that the heterojunction structure in these nanoparticles greatly enhances the generation of long-lived charges (millisecond to second timescale) even in the absence of electron/hole scavengers or Pt. Such long-lived reactive charges open potential applications in water-splitting Z-schemes and in driving kinetically slow and technologically desirable oxidations.

Original language	English (US)
Pages (from-to)	340-351
Number of pages	12
Journal	NATURE ENERGY
Volume	7
Issue number	4
DOIs	https://doi.org/10.1038/s41560-022-00990-2
State	Published - Apr 2022

Bibliographical note

Funding Information:
We acknowledge financial support from KAUST, including Office of Sponsored Research (OSR) awards no. OSR-2019-CRG8-4086 IED-OSR-2019-4454 (I.M.) and OSR-2018-CRG7-3749 (I.M.). We acknowledge funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 952911, project BOOSTER (I.M.), grant agreement no. 862474, project RoLA-FLEX (I.M.), and grant agreement no. 101007084, project CITYSOLAR (IM), as well as EPSRC Project EP/T026219/1 (I.M.). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement no. 886664 (S.G-C).

Publisher Copyright:
© 2022, The Author(s), under exclusive licence to Springer Nature Limited.

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1038/s41560-022-00990-2

Cite this

Kosco, J., Gonzalez-Carrero, S., Howells, C. T., Fei, T., Dong, Y., Sougrat, R., Harrison, G. T., Firdaus, Y., Sheelamanthula, R., Purushothaman, B., Moruzzi, F., Xu, W., Zhao, L., Basu, A., De Wolf, S., Anthopoulos, T. D., Durrant, J. R., & McCulloch, I. (2022). Generation of long-lived charges in organic semiconductor heterojunction nanoparticles for efficient photocatalytic hydrogen evolution. NATURE ENERGY, 7(4), 340-351. https://doi.org/10.1038/s41560-022-00990-2

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title = "Generation of long-lived charges in organic semiconductor heterojunction nanoparticles for efficient photocatalytic hydrogen evolution",

abstract = "Organic semiconductor photocatalysts for the production of solar fuels are attractive as they can be synthetically tuned to absorb visible light while simultaneously retaining suitable energy levels to drive a range of processes. However, a greater understanding of the photophysics that determines the function of organic semiconductor heterojunction nanoparticles is needed to optimize performance. Here, we show that such materials can intrinsically generate remarkably long-lived reactive charges, enabling them to efficiently drive sacrificial hydrogen evolution. Our optimized hetereojunction photocatalysts comprise the conjugated polymer PM6 matched with Y6 or PCBM electron acceptors, and achieve external quantum efficiencies of 1.0% to 5.0% at 400 to 900 nm and 8.7% to 2.6% at 400 to 700 nm, respectively. Employing transient and operando spectroscopies, we find that the heterojunction structure in these nanoparticles greatly enhances the generation of long-lived charges (millisecond to second timescale) even in the absence of electron/hole scavengers or Pt. Such long-lived reactive charges open potential applications in water-splitting Z-schemes and in driving kinetically slow and technologically desirable oxidations.",

author = "Jan Kosco and Soranyel Gonzalez-Carrero and Howells, {Calvyn T.} and Teng Fei and Yifan Dong and Rachid Sougrat and Harrison, {George T.} and Yuliar Firdaus and Rajendar Sheelamanthula and Balaji Purushothaman and Floriana Moruzzi and Weidong Xu and Lingyun Zhao and Aniruddha Basu and {De Wolf}, Stefaan and Anthopoulos, {Thomas D.} and Durrant, {James R.} and Iain McCulloch",

note = "Funding Information: We acknowledge financial support from KAUST, including Office of Sponsored Research (OSR) awards no. OSR-2019-CRG8-4086 IED-OSR-2019-4454 (I.M.) and OSR-2018-CRG7-3749 (I.M.). We acknowledge funding from the European Union{\textquoteright}s Horizon 2020 research and innovation programme under grant agreement no. 952911, project BOOSTER (I.M.), grant agreement no. 862474, project RoLA-FLEX (I.M.), and grant agreement no. 101007084, project CITYSOLAR (IM), as well as EPSRC Project EP/T026219/1 (I.M.). This project has received funding from the European Union{\textquoteright}s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement no. 886664 (S.G-C). Publisher Copyright: {\textcopyright} 2022, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2022",

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doi = "10.1038/s41560-022-00990-2",

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Kosco, J, Gonzalez-Carrero, S, Howells, CT, Fei, T, Dong, Y, Sougrat, R, Harrison, GT, Firdaus, Y, Sheelamanthula, R, Purushothaman, B, Moruzzi, F, Xu, W, Zhao, L, Basu, A, De Wolf, S, Anthopoulos, TD, Durrant, JR & McCulloch, I 2022, 'Generation of long-lived charges in organic semiconductor heterojunction nanoparticles for efficient photocatalytic hydrogen evolution', NATURE ENERGY, vol. 7, no. 4, pp. 340-351. https://doi.org/10.1038/s41560-022-00990-2

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AU - Gonzalez-Carrero, Soranyel

AU - Howells, Calvyn T.

AU - Fei, Teng

AU - Dong, Yifan

AU - Sougrat, Rachid

AU - Harrison, George T.

AU - Firdaus, Yuliar

AU - Sheelamanthula, Rajendar

AU - Purushothaman, Balaji

AU - Moruzzi, Floriana

AU - Xu, Weidong

AU - Zhao, Lingyun

AU - Basu, Aniruddha

AU - De Wolf, Stefaan

AU - Anthopoulos, Thomas D.

AU - Durrant, James R.

AU - McCulloch, Iain

N1 - Funding Information: We acknowledge financial support from KAUST, including Office of Sponsored Research (OSR) awards no. OSR-2019-CRG8-4086 IED-OSR-2019-4454 (I.M.) and OSR-2018-CRG7-3749 (I.M.). We acknowledge funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 952911, project BOOSTER (I.M.), grant agreement no. 862474, project RoLA-FLEX (I.M.), and grant agreement no. 101007084, project CITYSOLAR (IM), as well as EPSRC Project EP/T026219/1 (I.M.). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement no. 886664 (S.G-C). Publisher Copyright: © 2022, The Author(s), under exclusive licence to Springer Nature Limited.

PY - 2022/4

Y1 - 2022/4

N2 - Organic semiconductor photocatalysts for the production of solar fuels are attractive as they can be synthetically tuned to absorb visible light while simultaneously retaining suitable energy levels to drive a range of processes. However, a greater understanding of the photophysics that determines the function of organic semiconductor heterojunction nanoparticles is needed to optimize performance. Here, we show that such materials can intrinsically generate remarkably long-lived reactive charges, enabling them to efficiently drive sacrificial hydrogen evolution. Our optimized hetereojunction photocatalysts comprise the conjugated polymer PM6 matched with Y6 or PCBM electron acceptors, and achieve external quantum efficiencies of 1.0% to 5.0% at 400 to 900 nm and 8.7% to 2.6% at 400 to 700 nm, respectively. Employing transient and operando spectroscopies, we find that the heterojunction structure in these nanoparticles greatly enhances the generation of long-lived charges (millisecond to second timescale) even in the absence of electron/hole scavengers or Pt. Such long-lived reactive charges open potential applications in water-splitting Z-schemes and in driving kinetically slow and technologically desirable oxidations.

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Generation of long-lived charges in organic semiconductor heterojunction nanoparticles for efficient photocatalytic hydrogen evolution

Abstract

Bibliographical note

ASJC Scopus subject areas

UN SDGs

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