Revealing the aging process of solid electrolyte interphase on SiOx anode

Guoyu Qian, Yiwei Li, Haibiao Chen, Lin Xie, Tongchao Liu, Ni Yang, Yongli Song, Cong Lin, Junfang Cheng, Naotoshi Nakashima, Meng Zhang, Zikun Li, Wenguang Zhao, Xiangjie Yang, Hai Lin, Xia Lu, Luyi Yang (), Hong Li, Khalil Amine, Liquan Chen and Feng Pan ()
Additional contact information
Guoyu Qian: Peking University, Shenzhen Graduate School
Yiwei Li: Peking University, Shenzhen Graduate School
Haibiao Chen: Peking University, Shenzhen Graduate School
Lin Xie: Southern University of Science and Technology
Tongchao Liu: Argonne National Laboratory
Ni Yang: Peking University, Shenzhen Graduate School
Yongli Song: Peking University, Shenzhen Graduate School
Cong Lin: Peking University, Shenzhen Graduate School
Junfang Cheng: Kyushu University
Naotoshi Nakashima: Kyushu University
Meng Zhang: BTR New Material Group Co., Ltd
Zikun Li: BTR New Material Group Co., Ltd
Wenguang Zhao: Peking University, Shenzhen Graduate School
Xiangjie Yang: Sun Yat-sen University
Hai Lin: Peking University, Shenzhen Graduate School
Xia Lu: Sun Yat-sen University
Luyi Yang: Peking University, Shenzhen Graduate School
Hong Li: Chinese Academy of Sciences
Khalil Amine: Argonne National Laboratory
Liquan Chen: Chinese Academy of Sciences
Feng Pan: Peking University, Shenzhen Graduate School

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract As one of the most promising alternatives to graphite negative electrodes, silicon oxide (SiOx) has been hindered by its fast capacity fading. Solid electrolyte interphase (SEI) aging on silicon SiOx has been recognized as the most critical yet least understood facet. Herein, leveraging 3D focused ion beam-scanning electron microscopy (FIB-SEM) tomographic imaging, we reveal an exceptionally characteristic SEI microstructure with an incompact inner region and a dense outer region, which overturns the prevailing belief that SEIs are homogeneous structure and reveals the SEI evolution process. Through combining nanoprobe and electron energy loss spectroscopy (EELS), it is also discovered that the electronic conductivity of thick SEI relies on the percolation network within composed of conductive agents (e.g., carbon black particles), which are embedded into the SEI upon its growth. Therefore, the free growth of SEI will gradually attenuate this electron percolation network, thereby causing capacity decay of SiOx. Based on these findings, a proof-of-concept strategy is adopted to mechanically restrict the SEI growth via applying a confining layer on top of the electrode. Through shedding light on the fundamental understanding of SEI aging for SiOx anodes, this work could potentially inspire viable improving strategies in the future.

Date: 2023
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DOI: 10.1038/s41467-023-41867-6

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