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Weihua Lin. Portrait.

Weihua Lin

Postdoctoral fellow

Weihua Lin. Portrait.

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

Author

  • Qian Zhao
  • Mohamed Abdellah
  • Yuehan Cao
  • Jie Meng
  • Xianshao Zou
  • Kasper Ene-mark-Rasmussen
  • Weihua Lin
  • Yi Li
  • Yijiang Chen
  • Hengli Duan
  • Qinying Pan
  • Ying Zhou
  • Tonu Pullerits
  • Hong Xu
  • Sophie E. Canton
  • Yuran Niu
  • Kaibo Zheng
Show all

Summary, in English

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.

Department/s

  • LU Profile Area: Light and Materials
  • Chemical Physics
  • NanoLund: Centre for Nanoscience
  • LTH Profile Area: Nanoscience and Semiconductor Technology
  • LTH Profile Area: Photon Science and Technology
  • MAX IV Laboratory

Publishing year

2024

Language

English

Publication/Series

Advanced Functional Materials

Volume

34

Issue

30

Document type

Journal article

Publisher

Wiley-Blackwell

Topic

  • Physical Chemistry (including Surface- and Colloid Chemistry)

Keywords

  • methane
  • multi-electron donation
  • photocatalytic reduction of CO
  • quantum dot
  • size-dependent

Status

Published

ISBN/ISSN/Other

  • ISSN: 1616-301X