Templated 2D polymer heterojunctions for improved photocatalytic hydrogen production
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 material...
| Những tác giả chính: | , , , , , , , , , , , , |
|---|---|
| Định dạng: | Journal article |
| Ngôn ngữ: | English |
| Được phát hành: |
Wiley
2023
|
| _version_ | 1826313752268505088 |
|---|---|
| author | Aitchison, CM Gonzalez-Carrero, S Yao, S Benkert, M Ding, Z Young, NP Willner, B Moruzzi, F Lin, Y Tian, J Nellist, PD Durrant, JR McCulloch, I |
| author_facet | Aitchison, CM Gonzalez-Carrero, S Yao, S Benkert, M Ding, Z Young, NP Willner, B Moruzzi, F Lin, Y Tian, J Nellist, PD Durrant, JR McCulloch, I |
| author_sort | Aitchison, CM |
| collection | OXFORD |
| description | 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<sup>−1</sup> m<sup>−2</sup> 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. |
| first_indexed | 2024-03-07T08:06:01Z |
| format | Journal article |
| id | oxford-uuid:0db33374-9ffd-4a47-9948-ae1b196c156d |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-09-25T04:19:52Z |
| publishDate | 2023 |
| publisher | Wiley |
| record_format | dspace |
| spelling | oxford-uuid:0db33374-9ffd-4a47-9948-ae1b196c156d2024-08-08T11:06:47ZTemplated 2D polymer heterojunctions for improved photocatalytic hydrogen productionJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:0db33374-9ffd-4a47-9948-ae1b196c156dEnglishSymplectic ElementsWiley2023Aitchison, CMGonzalez-Carrero, SYao, SBenkert, MDing, ZYoung, NPWillner, BMoruzzi, FLin, YTian, JNellist, PDDurrant, JRMcCulloch, I2D 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<sup>−1</sup> m<sup>−2</sup> 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. |
| spellingShingle | Aitchison, CM Gonzalez-Carrero, S Yao, S Benkert, M Ding, Z Young, NP Willner, B Moruzzi, F Lin, Y Tian, J Nellist, PD Durrant, JR McCulloch, I Templated 2D polymer heterojunctions for improved photocatalytic hydrogen production |
| title | Templated 2D polymer heterojunctions for improved photocatalytic hydrogen production |
| title_full | Templated 2D polymer heterojunctions for improved photocatalytic hydrogen production |
| title_fullStr | Templated 2D polymer heterojunctions for improved photocatalytic hydrogen production |
| title_full_unstemmed | Templated 2D polymer heterojunctions for improved photocatalytic hydrogen production |
| title_short | Templated 2D polymer heterojunctions for improved photocatalytic hydrogen production |
| title_sort | templated 2d polymer heterojunctions for improved photocatalytic hydrogen production |
| work_keys_str_mv | AT aitchisoncm templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT gonzalezcarreros templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT yaos templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT benkertm templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT dingz templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT youngnp templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT willnerb templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT moruzzif templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT liny templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT tianj templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT nellistpd templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT durrantjr templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction AT mccullochi templated2dpolymerheterojunctionsforimprovedphotocatalytichydrogenproduction |