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...

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Main Authors: Zhaoqi Shen, Yujie Zhang, Guang Zhang, Shiyong Liu
Format: Article
Language:English
Published: MDPI AG 2023-11-01
Series:Molecules
Subjects:
Online Access:https://www.mdpi.com/1420-3049/28/22/7500
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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.
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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