Depth-Dependent Understanding of Cathode Electrolyte Interphase (CEI) on the Layered Li-Ion Cathodes Operated at Extreme High Temperature

Nagarajan, Sudhan; Weiland, Conan; Hwang, Sooyeon; Balasubramanian, Mahalingam; Arava, Leela Reddy

doi:10.1021/acs.chemmater.2c00435

Depth-Dependent Understanding of Cathode Electrolyte Interphase (CEI) on the Layered Li-Ion Cathodes Operated at Extreme High Temperature

Journal Article · Tue May 03 00:00:00 EDT 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.2c00435· OSTI ID:1867192

^[1]; Weiland, Conan ^[2]; ^[3]; ^[4]; ^[1]

Wayne State Univ., Detroit, MI (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Material Measurement Lab.
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)

The high-temperature operation of Li-ion batteries is highly dependent on the stability of the cathode electrolyte interphase (CEI) formed during lithiation-delithiation reactions. However, knowledge on the nature of the CEI is limited and its stability under extreme temperatures is not well understood. Therefore, herein, we investigate a proof-of-concept study on stabilizing CEI on model LiNi_0.33Mn_0.33Co_0.33O₂ (NMC333) at extreme operation condition of 100 oC using thermally stable pyrrolidinium based ionic liquid electrolyte. The electrochemical lithiation-delithiation reactions at 100 oC and the CEI evolution upon different cycling conditions are investigated. Further, the depth-dependent CEI chemistry was investigated using energy tunable synchrotron-based hard X-ray photoelectron spectroscopy (HAXPES). Overall, the results reveal that the high temperature operation accelerated the CEI formation compared to room temperature, and the surface of the interphase layer is rich in boron-based inorganic moieties than the deeper surface. Further, bulk sensitive X-ray absorption spectroscopy (XAS) was used to investigate the transition metal redox contributors during high temperature electrochemical reactions, similar to room temperature, the Ni2+/4+redox couple is the only charge compensating redox couple during high temperature operation. Finally, the physical nature of the conformal CEI on the cathode particles was visualized with high-resolution transmission electron microscopy, which confirms that the significant degradation of cathode particles without conformal CEI is due to the transformation of layer to spinel formation at extreme temperature. In this study, understanding this high temperature interfacial chemistry of NMC cathodes through advanced spectroscopy and microscopy will shed light on transforming ambient temperature Li-ion chemistry to high temperature applications.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 1867192

Alternate ID(s):: OSTI ID: 1960729

Report Number(s):: BNL-222983-2022-JAAM

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 10 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Depth-Dependent Understanding of Cathode Electrolyte Interphase (CEI) on the Layered Li-Ion Cathodes Operated at Extreme High Temperature

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