Ultrafast charge transfer dynamics in 2D covalent organic frameworks/Re-complex hybrid photocatalyst

Qinying Pan, Mohamed Abdellah (), Yuehan Cao, Weihua Lin, Yang Liu, Jie Meng, Quan Zhou, Qian Zhao, Xiaomei Yan, Zonglong Li, Hao Cui, Huili Cao, Wenting Fang, David Ackland Tanner, Mahmoud Abdel-Hafiez, Ying Zhou (), Tonu Pullerits, Sophie E. Canton, Hong Xu () and Kaibo Zheng ()
Additional contact information
Qinying Pan: Technical University of Denmark
Mohamed Abdellah: Chemical Physics and NanoLund, Lund University
Yuehan Cao: State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University
Weihua Lin: Chemical Physics and NanoLund, Lund University
Yang Liu: State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University
Jie Meng: Technical University of Denmark
Quan Zhou: Technical University of Denmark
Qian Zhao: Technical University of Denmark
Xiaomei Yan: Technical University of Denmark
Zonglong Li: Institute of Nuclear and New Energy Technology, Tsinghua University
Hao Cui: Institute of Nuclear and New Energy Technology, Tsinghua University
Huili Cao: Technical University of Denmark
Wenting Fang: Technical University of Denmark
David Ackland Tanner: Technical University of Denmark
Mahmoud Abdel-Hafiez: Uppsala University
Ying Zhou: State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University
Tonu Pullerits: Chemical Physics and NanoLund, Lund University
Sophie E. Canton: European XFEL
Hong Xu: Institute of Nuclear and New Energy Technology, Tsinghua University
Kaibo Zheng: Technical University of Denmark

Nature Communications, 2022, vol. 13, issue 1, 1-13

Abstract: Abstract Rhenium(I)-carbonyl-diimine complexes have emerged as promising photocatalysts for carbon dioxide reduction with covalent organic frameworks recognized as perfect sensitizers and scaffold support. Such Re complexes/covalent organic frameworks hybrid catalysts have demonstrated high carbon dioxide reduction activities but with strong excitation energy-dependence. In this paper, we rationalize this behavior by the excitation energy-dependent pathways of internal photo-induced charge transfer studied via transient optical spectroscopies and time-dependent density-functional theory calculation. Under band-edge excitation, the excited electrons are quickly injected from covalent organic frameworks moiety into catalytic RheniumI center within picosecond but followed by fast backward geminate recombination. While under excitation with high-energy photon, the injected electrons are located at high-energy levels in RheniumI centers with longer lifetime. Besides those injected electrons to RheniumI center, there still remain some long-lived electrons in covalent organic frameworks moiety which is transferred back from RheniumI. This facilitates the two-electron reaction of carbon dioxide conversion to carbon monoxide.

Date: 2022
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DOI: 10.1038/s41467-022-28409-2

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