Photocatalytic Oxygen Evolution under Visible Light Mediated by Molecular Heterostructures
Due to their structural and property tunability, semiconductive conjugated polymers (CPs) have emerged as promising candidates for photocatalytic water splitting. Compared with inorganic materials, the photocatalytic performance of mono-component polymers was limited by the fast recombination of pho...
Main Authors: | , , , |
---|---|
Format: | Article |
Language: | English |
Published: |
MDPI AG
2023-11-01
|
Series: | Molecules |
Subjects: | |
Online Access: | https://www.mdpi.com/1420-3049/28/22/7500 |
_version_ | 1827639149561118720 |
---|---|
author | Zhaoqi Shen Yujie Zhang Guang Zhang Shiyong Liu |
author_facet | Zhaoqi Shen Yujie Zhang Guang Zhang Shiyong Liu |
author_sort | Zhaoqi Shen |
collection | DOAJ |
description | Due to their structural and property tunability, semiconductive conjugated polymers (CPs) have emerged as promising candidates for photocatalytic water splitting. Compared with inorganic materials, the photocatalytic performance of mono-component polymers was limited by the fast recombination of photoexcited charge carriers, and they always needed to catch up to expectations. To this end, researchers established molecular donor–acceptor heterostructures, which could notably promote oxygen production efficiency due to their more effective charge carrier separation. In this work, easy Schiff base reactions between side-chain -CHO groups and terminal -NH<sub>2</sub> groups were used to introduce benzene and perylene diimide (PDI) into the molecular heterostructure to serve as electron donors (D) and electron acceptors (A). In particular, for the first time, we employed the molecular heterostructures of CPs to promote photocatalytic O<sub>2</sub> production. One prepared molecular heterostructure was demonstrated to improve oxygen generation rate (up to 0.53 mmol g<sup>−1</sup> h<sup>−1</sup>) through visible light-driven water splitting. Interestingly, based on the photoelectric properties, a stepwise two-electron/two-electron pathway constituted the photocatalytic mechanism for oxygen production with the molecular heterostructure. These results provide insights into designing and fabricating high-performance molecular heterostructures for photocatalytic oxygen production. |
first_indexed | 2024-03-09T16:34:35Z |
format | Article |
id | doaj.art-b283f83d20dc4bc78501de3859b77832 |
institution | Directory Open Access Journal |
issn | 1420-3049 |
language | English |
last_indexed | 2024-03-09T16:34:35Z |
publishDate | 2023-11-01 |
publisher | MDPI AG |
record_format | Article |
series | Molecules |
spelling | doaj.art-b283f83d20dc4bc78501de3859b778322023-11-24T14:57:57ZengMDPI AGMolecules1420-30492023-11-012822750010.3390/molecules28227500Photocatalytic Oxygen Evolution under Visible Light Mediated by Molecular HeterostructuresZhaoqi Shen0Yujie Zhang1Guang Zhang2Shiyong Liu3School of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaSchool of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaDepartment of Chemistry, Tianjin University, Tianjin 300072, ChinaSchool of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, ChinaDue to their structural and property tunability, semiconductive conjugated polymers (CPs) have emerged as promising candidates for photocatalytic water splitting. Compared with inorganic materials, the photocatalytic performance of mono-component polymers was limited by the fast recombination of photoexcited charge carriers, and they always needed to catch up to expectations. To this end, researchers established molecular donor–acceptor heterostructures, which could notably promote oxygen production efficiency due to their more effective charge carrier separation. In this work, easy Schiff base reactions between side-chain -CHO groups and terminal -NH<sub>2</sub> groups were used to introduce benzene and perylene diimide (PDI) into the molecular heterostructure to serve as electron donors (D) and electron acceptors (A). In particular, for the first time, we employed the molecular heterostructures of CPs to promote photocatalytic O<sub>2</sub> production. One prepared molecular heterostructure was demonstrated to improve oxygen generation rate (up to 0.53 mmol g<sup>−1</sup> h<sup>−1</sup>) through visible light-driven water splitting. Interestingly, based on the photoelectric properties, a stepwise two-electron/two-electron pathway constituted the photocatalytic mechanism for oxygen production with the molecular heterostructure. These results provide insights into designing and fabricating high-performance molecular heterostructures for photocatalytic oxygen production.https://www.mdpi.com/1420-3049/28/22/7500perylene diimidemolecular heterostructuresoxygen evolution rate |
spellingShingle | Zhaoqi Shen Yujie Zhang Guang Zhang Shiyong Liu Photocatalytic Oxygen Evolution under Visible Light Mediated by Molecular Heterostructures Molecules perylene diimide molecular heterostructures oxygen evolution rate |
title | Photocatalytic Oxygen Evolution under Visible Light Mediated by Molecular Heterostructures |
title_full | Photocatalytic Oxygen Evolution under Visible Light Mediated by Molecular Heterostructures |
title_fullStr | Photocatalytic Oxygen Evolution under Visible Light Mediated by Molecular Heterostructures |
title_full_unstemmed | Photocatalytic Oxygen Evolution under Visible Light Mediated by Molecular Heterostructures |
title_short | Photocatalytic Oxygen Evolution under Visible Light Mediated by Molecular Heterostructures |
title_sort | photocatalytic oxygen evolution under visible light mediated by molecular heterostructures |
topic | perylene diimide molecular heterostructures oxygen evolution rate |
url | https://www.mdpi.com/1420-3049/28/22/7500 |
work_keys_str_mv | AT zhaoqishen photocatalyticoxygenevolutionundervisiblelightmediatedbymolecularheterostructures AT yujiezhang photocatalyticoxygenevolutionundervisiblelightmediatedbymolecularheterostructures AT guangzhang photocatalyticoxygenevolutionundervisiblelightmediatedbymolecularheterostructures AT shiyongliu photocatalyticoxygenevolutionundervisiblelightmediatedbymolecularheterostructures |