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In-situ formatting donor-acceptor polymer with giant dipole moment and ultrafast exciton separation

Chang Cheng, Jiaguo Yu (), Difa Xu, Lei Wang, Guijie Liang, Liuyang Zhang () and Mietek Jaroniec ()
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Chang Cheng: State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology
Jiaguo Yu: State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology
Difa Xu: Hunan Key Laboratory of Applied Environmental Photocatalysis, Changsha University
Lei Wang: Hubei Key Laboratory of Low Dimensional Optoelectronic Material and Devices, Hubei University of Arts and Science
Guijie Liang: Hubei Key Laboratory of Low Dimensional Optoelectronic Material and Devices, Hubei University of Arts and Science
Liuyang Zhang: China University of Geosciences
Mietek Jaroniec: Kent State University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Donor-acceptor semiconducting polymers present countless opportunities for application in photocatalysis. Previous studies have showcased their advantages through direct bottom-up methods. Unfortunately, these approaches often involve harsh reaction conditions, overlooking the impact of uncontrolled polymerization degrees on photocatalysis. Besides, the mechanism behind the separation of electron-hole pairs (excitons) in donor-acceptor polymers remains elusive. This study presents a post-synthetic method involving the light-induced transformation of the building blocks of hyper-cross-linked polymers from donor-carbon-donor to donor-carbon-acceptor states, resulting in a polymer with a substantial intramolecular dipole moment. Thus, excitons are efficiently separated in the transformed polymer. The utility of this strategy is exemplified by the enhanced photocatalytic hydrogen peroxide synthesis. Encouragingly, our observations reveal the formation of intramolecular charge transfer states using time-resolved techniques, confirming transient exciton behavior involving separation and relaxation. This light-induced method not only guides the development of highly efficient donor-acceptor polymer photocatalysts but also applies to various fields, including organic solar cells, light-emitting diodes, and sensors.

Date: 2024
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DOI: 10.1038/s41467-024-45604-5

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