Understanding the Effect of Cathode Composition on the Interface and Crosstalk in NMC/Si Full Cells

Minkyu Kim; Zhenzhen Yang; Stephen E Trask; Ira Bloom

doi:10.1021/acsami.1c22364

Understanding the Effect of Cathode Composition on the Interface and Crosstalk in NMC/Si Full Cells

ACS Appl Mater Interfaces. 2022 Apr 6;14(13):15103-15111. doi: 10.1021/acsami.1c22364. Epub 2022 Mar 28.

Authors

Minkyu Kim^{1

2}, Zhenzhen Yang¹, Stephen E Trask¹, Ira Bloom¹

Affiliations

¹ Chemical Science and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States.
² Department of Chemistry, Inha University, 100 Inha-ro, Michuhol-gu, Incheon 22212, Republic of Korea.

PMID: 35343672
DOI: 10.1021/acsami.1c22364

Abstract

Crosstalk between the cathode and the anode in lithium-ion batteries has a great impact on performance, safety, and cycle lifetime. However, no report exists for a systematic investigation on crosstalk behavior in silicon (Si)-based cells as a function of transition metal composition in cathodes. We studied the effect of crosstalk on degradation of Si-rich anodes in full cells with different cathodes having the same crystal structure but different transition metal compositions, such as LiNi_1/3Mn_1/3Co_1/3O₂ (NM111), LiNi_0.5Mn_0.3Co_0.2O₂ (NMC532), and LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811). We found that the transition metal composition in cathodes, especially Mn ion concentration, significantly affects electrolyte decomposition reactions, even from very early cycles. This change causes differences in the solid electrolyte interphase (SEI) chemistry of each aged Si sample. As a result, each of the aged Si samples has a different electrochemistry, in terms of initial Coulombic efficiency and the mechanism of capacity fade.

Keywords: NMC cathodes; Si anode; crosstalk; solid electrolyte interphase (SEI); transition metal dissolution.