Impacts of Dissolved Ni2+ on the Solid Electrolyte Interphase on a Graphite Anode

Hanying Xu; Zhanping Li; Tongchao Liu; Ce Han; Chong Guo; He Zhao; Qin Li; Jun Lu; Khalil Amine; Xinping Qiu

doi:10.1002/anie.202202894

Impacts of Dissolved Ni²⁺ on the Solid Electrolyte Interphase on a Graphite Anode

Angew Chem Int Ed Engl. 2022 Jul 25;61(30):e202202894. doi: 10.1002/anie.202202894. Epub 2022 May 26.

Authors

Hanying Xu¹, Zhanping Li^{1

2}, Tongchao Liu³, Ce Han¹, Chong Guo², He Zhao¹, Qin Li², Jun Lu³, Khalil Amine^{3

4}, Xinping Qiu¹

Affiliations

¹ Key Laboratory of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University, Beijing, 100084, China.
² Analysis Center, Tsinghua University, Beijing, 100084, China.
³ Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 Cass Ave, Lemont, IL 60439, USA.
⁴ Department of Material Science and Engineering, Stanford University, Stanford, CA 94305, USA.

PMID: 35441399
DOI: 10.1002/anie.202202894

Abstract

Transition metal (e.g. Ni) ions dissolved from layered-structured Ni-rich cathodes can migrate to the anode side and accelerate the failure of lithium-ion batteries. The investigations of the impact and distribution of Ni species on the solid electrolyte interphase (SEI) on the anode are crucial to understand the failure mechanism. Herein, we used time-of-flight secondary ion mass spectroscopy (TOF-SIMS) coupled with multivariate curve resolution (MCR) analysis to intuitively characterize the distribution of Ni species in the SEI. We find that the SEI on the graphite electrode using an EC-based electrolyte exhibits a multi-stratum structure. During accelerated aging of the LiNi_0.88 Co_0.08 Mn_0.04 O₂ /graphite full cell, the dissolution of Ni aggravates significantly upon cycling. A strong correlation between the dissolved-Ni and organic species in the SEI on graphite is illustrated. The ion-exchange reaction between Ni²⁺ and Li⁺ ions in the SEI is demonstrated to be the main reason for the increase of SEI resistivity.

Keywords: Lithium-Ion Batteries; MCR Analysis; Ni Dissolution; SEI Structure; TOF-SIMS.

Abstract

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