Kim Minkyu, Yang Zhenzhen, Trask Stephen E, Bloom Ira
Chemical Science and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States.
Department of Chemistry, Inha University, 100 Inha-ro, Michuhol-gu, Incheon 22212, Republic of Korea.
ACS Appl Mater Interfaces. 2022 Apr 6;14(13):15103-15111. doi: 10.1021/acsami.1c22364. Epub 2022 Mar 28.
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 LiNiMnCoO (NM111), LiNiMnCoO (NMC532), and LiNiMnCoO (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.
锂离子电池中阴极和阳极之间的串扰对性能、安全性和循环寿命有很大影响。然而，目前尚无关于硅基电池中串扰行为随阴极过渡金属成分变化的系统研究报告。我们研究了串扰对全电池中富硅阳极降解的影响，这些全电池使用具有相同晶体结构但过渡金属成分不同的阴极，如LiNiMnCoO（NM111）、LiNiMnCoO（NMC532）和LiNiMnCoO（NMC811）。我们发现，阴极中的过渡金属成分，尤其是锰离子浓度，即使在非常早期的循环中也会显著影响电解质分解反应。这种变化导致每个老化硅样品的固体电解质界面（SEI）化学性质存在差异。结果，就初始库仑效率和容量衰减机制而言，每个老化硅样品都具有不同的电化学性质。
