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A paucity of redox centers, poor charge transport properties, and low structural stability of organic materials obstruct their use in practical applications. Herein, these issues have been addressed through the use of a redox-active salen-based framework polymer (RSFP) containing multiple redox-active centers in 𝝅-conjugated configuration for applications in lithium-ion batteries (LIBs). Based on its unique architecture, RSFP exhibits a superior reversible capacity of 671.8 mAh g−1 at 0.05 A g−1 after 168charge-discharge cycles. Importantly, the lithiation/de-lithiation performance is enhanced during operation, leading to an unprecedented reversible capacity of 946.2 mAh g−1 after 3500 cycles at 2 A g−1 . The structural evolution of RSFP is studied ex situ using X-ray photoelectron spectroscopy, revealing multiple active C═N, C─O, and C═O sites and aromatic sites such as benzene rings. Remarkably, the emergence of C═O originated from C─O is triggered by an electrochemical process, which is beneficial for improving reversible lithiation/delithiation behavior. Furthermore, the respective strong and weak binding interactions between redox centers and lithium ions, corresponding to theoretical capacities of 670.1 and 938.2 mAh g−1 , have been identified by density functional theory calculations manifesting14-electron redox reactions. This work sheds new light on routes for the development of redox-active organic materials for energy storage applications.

権利情報:

• Creative Commons BY Attribution 4.0 International
  

キーワード: Lithium ion storage, redox chemistry, redox-active framework polymer, storage mechanism, structural evolution

刊行年月日: 2024-03-25

出版者: Wiley

掲載誌:

• Small (ISSN: 16136810) vol. 20 issue. 28 2309321

研究助成金:

原稿種別: 出版者版 (Version of record)

MDR DOI:

公開URL: https://doi.org/10.1002/smll.202309321

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更新時刻: 2024-12-03 16:31:11 +0900

MDRでの公開時刻: 2024-12-03 16:31:11 +0900