Electron energy levels determining cathode electrolyte interphase formation

Zhang, Zhengfeng; Qin, Changdong; Cheng, Xiaopeng; Li, Jinhui; Zhang, Yuefei; Zhao, Wengao; Wang, Le; Du, Yingge; Sui, Manling; Yan, Pengfei

doi:10.1002/elt2.9

Electron energy levels determining cathode electrolyte interphase formation

Journal Article · Tue Oct 10 00:00:00 EDT 2023 · Electron

DOI:https://doi.org/10.1002/elt2.9· OSTI ID:2584260

Zhang, Zhengfeng ^[1]; Qin, Changdong ^[1]; Cheng, Xiaopeng ^[1]; Li, Jinhui ^[1]; Zhang, Yuefei ^[2]; Zhao, Wengao ^[3]; Wang, Le ^[4]; ^[4]; Sui, Manling ^[1]; ^[1]

Beijing University of Technology (China)
Zhejiang University, Hangzhou (China)
Karlsruhe Inst. of Technology (KIT), Eggenstein-Leopoldshafen (Germany)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Cathode electrolyte interphase (CEI) has a significant impact on the performance of rechargeable batteries and is gaining increasing attention. Understanding the fundamental and detailed CEI formation mechanism is of critical importance for battery chemistry. Herein, a diverse of characterization tools are utilized to comprehensively analyze the composition of the CEI layer as well as its formation mechanism by LiCoO₂ (LCO) cathode. We reveal that CEI is mainly composed of the reduction products of electrolyte and it only parasitizes the degraded LCO surface which has transformed into a disordered spinel structure due to oxygen loss and lithium depletion. Based on the energy diagram and the chemical potential analysis, the CEI formation process has been well explained, and the proposed CEI formation mechanism is further experimentally validated. This work highlights that the CEI formation process is nearly identical to that of the anode-electrolyte-interphase, both of which are generated due to the electrolyte directly in contact with the low chemical potential electrode material. This work can deepen and refresh our understanding of CEI.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2584260

Report Number(s):: PNNL-SA--186938

Journal Information:: Electron, Journal Name: Electron Journal Issue: 2 Vol. 1; ISSN 2751-2606; ISSN 2751-2614

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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