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Size-Dependent Multi-Electron Donation in Metal-Complex Quantum Dots Hybrid Catalyst for Photocatalytic Carbon Dioxide Reduction

Zhao, Qian ; Abdellah, Mohamed LU ; Cao, Yuehan ; Meng, Jie LU ; Zou, Xianshao LU ; Ene-mark-Rasmussen, Kasper ; Lin, Weihua LU ; Li, Yi ; Chen, Yijiang and Duan, Hengli , et al. (2024) In Advanced Functional Materials
Abstract

The effective conversion of carbon dioxide (CO2) into valuable chemical fuels relies significantly on the donation of multiple electrons. Its efficiency is closely linked to both the density and lifetime of excited charge carriers. In this study, a hybrid catalyst system comprising covalently bonded InP/ZnS quantum dots (QDs) and Re-complexes is showcased. The electronic band alignment between the QDs and the Re-complexes is revealed to dominate the multi-electron transfer process for photocatalytic conversion to methane (CH4). Notably, the size of the QDs is found to be a determining parameter. Among the three QD sizes investigated, transient absorption spectroscopy studies unveil that rapid multi-electron... (More)

The effective conversion of carbon dioxide (CO2) into valuable chemical fuels relies significantly on the donation of multiple electrons. Its efficiency is closely linked to both the density and lifetime of excited charge carriers. In this study, a hybrid catalyst system comprising covalently bonded InP/ZnS quantum dots (QDs) and Re-complexes is showcased. The electronic band alignment between the QDs and the Re-complexes is revealed to dominate the multi-electron transfer process for photocatalytic conversion to methane (CH4). Notably, the size of the QDs is found to be a determining parameter. Among the three QD sizes investigated, transient absorption spectroscopy studies unveil that rapid multi-electron transfer from the QDs to the Re-catalyst occurs in smaller QDs (2.3 nm) due to the substantial driving force. Consequently, the photocatalytic conversion of CO2 to CH4 is significantly enhanced with a turnover number of 6, corresponding to the overall apparent quantum yield of ≈1%. This research underscores the possibilities of engineering multi-electron transfer by manipulating the electronic band alignment within a catalytic system. This can serve as a guide for optimizing photocatalytic CO2 reduction.

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type
Contribution to journal
publication status
epub
subject
keywords
methane, multi-electron donation, photocatalytic reduction of CO, quantum dot, size-dependent
in
Advanced Functional Materials
publisher
Wiley-Blackwell
external identifiers
  • scopus:85189071596
ISSN
1616-301X
DOI
10.1002/adfm.202315734
language
English
LU publication?
yes
id
e4dee1bb-e958-404b-96b2-2b263edb6cb1
date added to LUP
2024-04-16 15:00:41
date last changed
2024-04-16 15:01:44
@article{e4dee1bb-e958-404b-96b2-2b263edb6cb1,
  abstract     = {{<p>The effective conversion of carbon dioxide (CO<sub>2</sub>) into valuable chemical fuels relies significantly on the donation of multiple electrons. Its efficiency is closely linked to both the density and lifetime of excited charge carriers. In this study, a hybrid catalyst system comprising covalently bonded InP/ZnS quantum dots (QDs) and Re-complexes is showcased. The electronic band alignment between the QDs and the Re-complexes is revealed to dominate the multi-electron transfer process for photocatalytic conversion to methane (CH<sub>4</sub>). Notably, the size of the QDs is found to be a determining parameter. Among the three QD sizes investigated, transient absorption spectroscopy studies unveil that rapid multi-electron transfer from the QDs to the Re-catalyst occurs in smaller QDs (2.3 nm) due to the substantial driving force. Consequently, the photocatalytic conversion of CO<sub>2</sub> to CH<sub>4</sub> is significantly enhanced with a turnover number of 6, corresponding to the overall apparent quantum yield of ≈1%. This research underscores the possibilities of engineering multi-electron transfer by manipulating the electronic band alignment within a catalytic system. This can serve as a guide for optimizing photocatalytic CO<sub>2</sub> reduction.</p>}},
  author       = {{Zhao, Qian and Abdellah, Mohamed and Cao, Yuehan and Meng, Jie and Zou, Xianshao and Ene-mark-Rasmussen, Kasper and Lin, Weihua and Li, Yi and Chen, Yijiang and Duan, Hengli and Pan, Qinying and Zhou, Ying and Pullerits, Tonu and Xu, Hong and Canton, Sophie E. and Niu, Yuran and Zheng, Kaibo}},
  issn         = {{1616-301X}},
  keywords     = {{methane; multi-electron donation; photocatalytic reduction of CO; quantum dot; size-dependent}},
  language     = {{eng}},
  publisher    = {{Wiley-Blackwell}},
  series       = {{Advanced Functional Materials}},
  title        = {{Size-Dependent Multi-Electron Donation in Metal-Complex Quantum Dots Hybrid Catalyst for Photocatalytic Carbon Dioxide Reduction}},
  url          = {{http://dx.doi.org/10.1002/adfm.202315734}},
  doi          = {{10.1002/adfm.202315734}},
  year         = {{2024}},
}