Two-Step Redox in Polyimide: Witness by In Situ Electron Paramagnetic Resonance in Lithium-ion Batteries

Bai, Yunfei1; Wang, Zhen1; Qin, Ning2; Ma, Detian1; Fu, Wenbin3; Lu, Zhouguang2; Pan, Xiaobo1

2023-03-01

10.1002/anie.202303162

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   Impact Factor & Quartile

1433-7851

1521-3773

Organic materials are promising candidates for future rechargeable batteries, owing to their high natural abundance and rapidly redox reaction. Elaborating the charge/discharge process of organic electrode is critical to unveil the fundamental redox mechanism of lithium-ion batteries (LIBs), but monitoring of this process is still challenging. Here, we report a nondestructive electron paramagnetic resonance (EPR) technique to real-time detect the electron migration step within polyimide cathode. From in situ EPR tests, we vividly observe a classical redox reaction along with two-electron transfer which only shows one pair of peaks in the cyclic voltammetry curve. The radical anion and dianion intermediates are detailed delineation at redox sites in EPR spectra, which can be further confirmed through density functional theory calculations. This approach is especially crucial to elaborate the correlation behind electrochemical and molecular structure for multistep organic-based LIBs.

Diamagnetic and Paramagnetic Species In Situ EPR Lithium-Ion Batteries Polyimide Electrode

SCI

English

Corresponding

National Natural Science Foundation of China["22171111","U22 A20439","21875097"] ; Basic Research Project of the Science and Technology Innovation Commission of Shenzhen[JCYJ20200109141640095] ; Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials[ZDSYS20200421111401738] ; Guangdong-Hong Kong-Macao Joint Laboratory[2019B121205001]

Chemistry

Chemistry, Multidisciplinary

WOS:000956917900001

WILEY-V C H VERLAG GMBH

CHEMISTRY

Web of Science

1.Lanzhou Univ, Coll Chem & Chem Engn, State Key Lab Appl Organ Chem, Key Lab Nonferrous Met Chem & Resources Utilizat G, Lanzhou 730000, Gansu, Peoples R China
2.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen Key Lab Interfacial Sci & Engn Mat, Guangdong Hong Kong Macao Joint Lab Photon Thermal, Shenzhen 518055, Guangdong, Peoples R China
3.Georgia Inst Technol, Sch Mat Sci & Engn, Atlanta, GA 30332 USA

Bai, Yunfei,Wang, Zhen,Qin, Ning,et al. Two-Step Redox in Polyimide: Witness by In Situ Electron Paramagnetic Resonance in Lithium-ion Batteries[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023.

Bai, Yunfei.,Wang, Zhen.,Qin, Ning.,Ma, Detian.,Fu, Wenbin.,...&Pan, Xiaobo.(2023).Two-Step Redox in Polyimide: Witness by In Situ Electron Paramagnetic Resonance in Lithium-ion Batteries.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION.

Bai, Yunfei,et al."Two-Step Redox in Polyimide: Witness by In Situ Electron Paramagnetic Resonance in Lithium-ion Batteries".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2023).