Templated 2D Polymer Heterojunctions for Improved Photocatalytic Hydrogen Production

Catherine M Aitchison; Soranyel Gonzalez-Carrero; Shilin Yao; Max Benkert; Zhiyuan Ding; Neil P. Young; Benjamin Willner; Floriana Moruzzi; Yuanbao Lin; Junfu Tian; Peter D. Nellist; James R. Durrant; Iain McCulloch

doi:10.1002/adma.202300037

Templated 2D Polymer Heterojunctions for Improved Photocatalytic Hydrogen Production

Catherine M Aitchison, Soranyel Gonzalez-Carrero, Shilin Yao, Max Benkert, Zhiyuan Ding, Neil P. Young, Benjamin Willner, Floriana Moruzzi, Yuanbao Lin, Junfu Tian, Peter D. Nellist, James R. Durrant, Iain McCulloch

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20 Scopus citations

Abstract

2D polymers have emerged as one of the most promising classes of organic photocatalysts for solar fuel production due to their tunability, charge-transport properties, and robustness. They are however difficult to process and so there are limited studies into the formation of heterojunction materials incorporating these components. In this work, a novel templating approach is used to combine an imine-based donor polymer and an acceptor polymer formed through Knoevenagel condensation. Heterojunction formation is shown to be highly dependent on the topological match of the donor and acceptor polymers with the most active templated material found to be between three and nine times more active for photocatalysis than its constituent components. Transient absorption spectroscopy reveals that this improvement is due to faster charge separation and more efficient charge extraction in the templated heterojunction. The templated material shows a very high hydrogen evolution rate of >20 mmol h−1 m−2 with an ascorbic acid hole scavenger but also produces hydrogen in the presence of only water and a cobalt-based redox mediator. This suggests the improved charge-separation interface and reduced trapping accessed through this approach could be suitable for Z-scheme formation.

Original language	English (US)
Journal	ADVANCED MATERIALS
DOIs	https://doi.org/10.1002/adma.202300037
State	Published - May 10 2023
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2023-06-20
Acknowledged KAUST grant number(s): CRG10
Acknowledgements: The authors would like to acknowledge financial support from KAUST Office of Sponsored Research CRG10, by EU Horizon 2020 grant agreement n°952911, BOOSTER, grant agreement n°862474, RoLA-FLEX, and grant agreement n°101007084 CITYSOLAR, as well as EPSRC Projects EP/T026219/1 and EP/W017091/1. This project received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement no. 886664 (S.G.-C.), and China Scholarhip Council-Imperial Scholarship (S.Y.). The authors acknowledge the David Cockayne Centre for Electron Microscopy at University of Oxford for access to equipment financially supported by the EPSRC (EP/K040375/1 “South of England Analytical Electron Microscope”) and the Henry Royce Institute for Advanced Materials (EP/R00661X/1, EP/S019367/1, EP/R010145/1).
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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10.1002/adma.202300037

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@article{cb1d6ef949494c0ab87f6c7006c63ce7,

title = "Templated 2D Polymer Heterojunctions for Improved Photocatalytic Hydrogen Production",

abstract = "2D polymers have emerged as one of the most promising classes of organic photocatalysts for solar fuel production due to their tunability, charge-transport properties, and robustness. They are however difficult to process and so there are limited studies into the formation of heterojunction materials incorporating these components. In this work, a novel templating approach is used to combine an imine-based donor polymer and an acceptor polymer formed through Knoevenagel condensation. Heterojunction formation is shown to be highly dependent on the topological match of the donor and acceptor polymers with the most active templated material found to be between three and nine times more active for photocatalysis than its constituent components. Transient absorption spectroscopy reveals that this improvement is due to faster charge separation and more efficient charge extraction in the templated heterojunction. The templated material shows a very high hydrogen evolution rate of >20 mmol h−1 m−2 with an ascorbic acid hole scavenger but also produces hydrogen in the presence of only water and a cobalt-based redox mediator. This suggests the improved charge-separation interface and reduced trapping accessed through this approach could be suitable for Z-scheme formation.",

author = "Aitchison, {Catherine M} and Soranyel Gonzalez-Carrero and Shilin Yao and Max Benkert and Zhiyuan Ding and Young, {Neil P.} and Benjamin Willner and Floriana Moruzzi and Yuanbao Lin and Junfu Tian and Nellist, {Peter D.} and Durrant, {James R.} and Iain McCulloch",

note = "KAUST Repository Item: Exported on 2023-06-20 Acknowledged KAUST grant number(s): CRG10 Acknowledgements: The authors would like to acknowledge financial support from KAUST Office of Sponsored Research CRG10, by EU Horizon 2020 grant agreement n°952911, BOOSTER, grant agreement n°862474, RoLA-FLEX, and grant agreement n°101007084 CITYSOLAR, as well as EPSRC Projects EP/T026219/1 and EP/W017091/1. This project received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement no. 886664 (S.G.-C.), and China Scholarhip Council-Imperial Scholarship (S.Y.). The authors acknowledge the David Cockayne Centre for Electron Microscopy at University of Oxford for access to equipment financially supported by the EPSRC (EP/K040375/1 “South of England Analytical Electron Microscope”) and the Henry Royce Institute for Advanced Materials (EP/R00661X/1, EP/S019367/1, EP/R010145/1). This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

year = "2023",

month = may,

day = "10",

doi = "10.1002/adma.202300037",

language = "English (US)",

journal = "ADVANCED MATERIALS",

issn = "1521-4095",

publisher = "Wiley",

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T1 - Templated 2D Polymer Heterojunctions for Improved Photocatalytic Hydrogen Production

AU - Aitchison, Catherine M

AU - Gonzalez-Carrero, Soranyel

AU - Yao, Shilin

AU - Benkert, Max

AU - Ding, Zhiyuan

AU - Young, Neil P.

AU - Willner, Benjamin

AU - Moruzzi, Floriana

AU - Lin, Yuanbao

AU - Tian, Junfu

AU - Nellist, Peter D.

AU - Durrant, James R.

AU - McCulloch, Iain

N1 - KAUST Repository Item: Exported on 2023-06-20 Acknowledged KAUST grant number(s): CRG10 Acknowledgements: The authors would like to acknowledge financial support from KAUST Office of Sponsored Research CRG10, by EU Horizon 2020 grant agreement n°952911, BOOSTER, grant agreement n°862474, RoLA-FLEX, and grant agreement n°101007084 CITYSOLAR, as well as EPSRC Projects EP/T026219/1 and EP/W017091/1. This project received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement no. 886664 (S.G.-C.), and China Scholarhip Council-Imperial Scholarship (S.Y.). The authors acknowledge the David Cockayne Centre for Electron Microscopy at University of Oxford for access to equipment financially supported by the EPSRC (EP/K040375/1 “South of England Analytical Electron Microscope”) and the Henry Royce Institute for Advanced Materials (EP/R00661X/1, EP/S019367/1, EP/R010145/1). This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2023/5/10

Y1 - 2023/5/10

N2 - 2D polymers have emerged as one of the most promising classes of organic photocatalysts for solar fuel production due to their tunability, charge-transport properties, and robustness. They are however difficult to process and so there are limited studies into the formation of heterojunction materials incorporating these components. In this work, a novel templating approach is used to combine an imine-based donor polymer and an acceptor polymer formed through Knoevenagel condensation. Heterojunction formation is shown to be highly dependent on the topological match of the donor and acceptor polymers with the most active templated material found to be between three and nine times more active for photocatalysis than its constituent components. Transient absorption spectroscopy reveals that this improvement is due to faster charge separation and more efficient charge extraction in the templated heterojunction. The templated material shows a very high hydrogen evolution rate of >20 mmol h−1 m−2 with an ascorbic acid hole scavenger but also produces hydrogen in the presence of only water and a cobalt-based redox mediator. This suggests the improved charge-separation interface and reduced trapping accessed through this approach could be suitable for Z-scheme formation.

AB - 2D polymers have emerged as one of the most promising classes of organic photocatalysts for solar fuel production due to their tunability, charge-transport properties, and robustness. They are however difficult to process and so there are limited studies into the formation of heterojunction materials incorporating these components. In this work, a novel templating approach is used to combine an imine-based donor polymer and an acceptor polymer formed through Knoevenagel condensation. Heterojunction formation is shown to be highly dependent on the topological match of the donor and acceptor polymers with the most active templated material found to be between three and nine times more active for photocatalysis than its constituent components. Transient absorption spectroscopy reveals that this improvement is due to faster charge separation and more efficient charge extraction in the templated heterojunction. The templated material shows a very high hydrogen evolution rate of >20 mmol h−1 m−2 with an ascorbic acid hole scavenger but also produces hydrogen in the presence of only water and a cobalt-based redox mediator. This suggests the improved charge-separation interface and reduced trapping accessed through this approach could be suitable for Z-scheme formation.

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UR - https://onlinelibrary.wiley.com/doi/10.1002/adma.202300037

UR - http://www.scopus.com/inward/record.url?scp=85161290477&partnerID=8YFLogxK

U2 - 10.1002/adma.202300037

DO - 10.1002/adma.202300037

M3 - Article

C2 - 37165538

SN - 1521-4095

JO - ADVANCED MATERIALS

JF - ADVANCED MATERIALS

ER -

Templated 2D Polymer Heterojunctions for Improved Photocatalytic Hydrogen Production

Abstract

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