Issue 37, 2022

Photoexcited charge manipulation in conjugated polymers bearing a Ru(ii) complex catalyst for visible-light CO2 reduction

Abstract

Conjugated polymers have emerged as promising candidates for photocatalyst materials. Design principles that maximize the synergy between the conjugated skeleton and catalyst moiety are strongly desired to be established for achieving efficient photocatalysis. Herein, the photoexcited charge manipulation was demonstrated by molecular engineering in conjugated polymers bearing a Ru(II) complex as the CO2 reduction photocatalyst. Combinational studies based on ultrafast spectroscopies and theoretical calculations revealed that the introduction of an electron-donating carbazole (Cz) skeleton in the polymer enables enhanced photoexcited charge trapping on the Ru(II)-complex catalyst moiety. The carbazole-based polymer [Cz-bpyRu]n facilitates CO2 reduction under visible light even longer than 500 nm and exhibited 7- to 15-fold greater activity than those of phenyl (Ph) and benzothiadiazole (Bt) counterparts. The findings of this study thus provide insights into molecular engineering for photoexcited charge manipulation to achieve efficient photocatalysis.

Graphical abstract: Photoexcited charge manipulation in conjugated polymers bearing a Ru(ii) complex catalyst for visible-light CO2 reduction

Supplementary files

Article information

Article type
Paper
Submitted
20 Marts 2022
Accepted
06 Maijs 2022
First published
09 Maijs 2022

J. Mater. Chem. A, 2022,10, 19821-19828

Author version available

Photoexcited charge manipulation in conjugated polymers bearing a Ru(II) complex catalyst for visible-light CO2 reduction

A. Nakada, R. Miyakawa, R. Itagaki, K. Kato, C. Takashima, A. Saeki, A. Yamakata, R. Abe, H. Nakai and H. Chang, J. Mater. Chem. A, 2022, 10, 19821 DOI: 10.1039/D2TA02183H

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