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In Situ and Real-Time Visualization of Mechanochemical Damage in Double-Network Hydrogels by Prefluorescent Probe via Oxygen-Relayed Radical Trapping

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Title: In Situ and Real-Time Visualization of Mechanochemical Damage in Double-Network Hydrogels by Prefluorescent Probe via Oxygen-Relayed Radical Trapping
Authors: Zheng, Yong Browse this author
Jiang, Julong Browse this author
Jin, Mingoo Browse this author →KAKEN DB
Miura, Daiyo Browse this author
Lu, Fei Xue Browse this author
Kubota, Koji Browse this author
Nakajima, Tasuku Browse this author →KAKEN DB
Maeda, Satoshi Browse this author →KAKEN DB
Ito, Hajime Browse this author →KAKEN DB
Gong, Jian Ping Browse this author →KAKEN DB
Issue Date: 5-Apr-2023
Publisher: American Chemical Society(ACS)
Journal Title: Journal of the American Chemical Society
Volume: 145
Issue: 13
Start Page: 7376
End Page: 7389
Publisher DOI: 10.1021/jacs.2c13764
Abstract: Visualization of mechanochemical damages, espe-cially for those in the molecular-scale (e.g., bond scission in polymeric materials), is of great industrial and academic significance. Herein, we report a novel strategy for in situ and real-time visualization of mechanochemical damages in hydrogels by utilizing prefluorescent probes via oxygen-relayed free-radical trapping. Double-network (DN) hydrogels that generate numerous mechanoradicals by homolytic bond scission of the brittle first network at large deformation are used as model materials. Theoretical calculation suggests that mechanoradicals generated by the damage of the first network undergo an oxygen-relayed radical-transfer process which can be detected by the prefluor-escent probe through the radical−radical coupling reaction. Such an oxygen-relayed radical-trapping process of the prefluorescent probe exhibits a dramatically enhanced emission, which enables the real-time sensing and visualization of mechanochemical damages in DN hydrogels made from brittle networks of varied chemical structures. To the best of authors’ knowledge, this work is the first report utilizing oxygen as a radical-relaying molecule for visualizing mechanoradical damages in polymer materials. Moreover, this new method based on the probe post-loading is simple and does not introduce any chemical structural changes in the materials, outperforming most previous methods that require chemical incorporation of mechanophores into polymer networks.
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright c American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Type: article (author version)
Appears in Collections:生命科学院・先端生命科学研究院 (Graduate School of Life Science / Faculty of Advanced Life Science) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 龔 剣萍 (Gong Jian Ping)

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