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Developing in situ electron paramagnetic resonance characterization for understanding electron transfer of rechargeable batteries

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Abstract

Electrochemical energy storage devices are pivotal in achieving “carbon neutrality” by enabling the storage of energy generated from renewable sources. To facilitate the development of these devices, it is important to gain insight into the underlying the single-/multi-electron transfer process. This can be achieved through in-time detection under operational conditions, but there are limited tools available for monitoring electron transfer under operando conditions. Electron paramagnetic resonance (EPR) is a powerful technique that can meet these expectations, as it is highly sensitive to unpaired electrons and can detect changes of paramagnetic centres. Despite the long history of in situ electrochemical EPR research, its potential has been surprisingly underutilized due to the need for strict operando cell design under special testing conditions. This review comprehensively summarizes recent efforts to understand energy storage mechanisms using in situ/operando EPR, with the aim of drawing researchers’ attention to this powerful technique. After introducing the fundamental principles of EPR, we describe the critical advances made in detecting batteries using operando EPR, along with the remaining challenges and opportunities for future development of this technology in batteries. We emphasize the need for strict operando cell design and the importance of designing experiments that closely mimic real-world conditions. We believe that this review will provide innovative solutions to solve tough problems that researchers may encounter during their battery research, and ultimately contribute to the development of more efficient and sustainable energy storage devices.

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Acknowledgements

The authors acknowledge the financial support from the National Natural Science Foundation of China (Nos. 22179145, 21975287, and 22138013), Taishan Scholars Program of Shandong Province (No. tsqn20221117), the startup support grant from China University of Petroleum (East China) (No. 27RA2204027), Shandong Provincial Natural Science Foundation (No. ZR2020ZD08), Shandong Province Postdoctoral Innovative Talent Support Program (No. SDBX2022034), and Qingdao Postdoctoral Innovation Project (No. QDBSH20220202003).

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  1. State Key Lab of Heavy Oil Processing, Institute of New Energy, College of Chemical Engineering, China University of Petroleum (East China), Qingdao, 266580, China

    Bin Wang, Wanli Wang, Yujie Xu, Yi Sun, Han Hu & Mingbo Wu

  2. Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry, Nanjing, 210042, China

    Kang Sun

  3. College of Physics, Qingdao University, Qingdao, 266071, China

    Qiang Li

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  1. Bin Wang
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Wang, B., Wang, W., Sun, K. et al. Developing in situ electron paramagnetic resonance characterization for understanding electron transfer of rechargeable batteries. Nano Res. 16, 11992–12012 (2023). https://doi.org/10.1007/s12274-023-5855-z

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