Acid- and Gas-Scavenging Electrolyte Additive Improving the Electrochemical Reversibility of Ni-Rich Cathodes in Li-Ion Batteries,ACS Applied Materials & Interfaces

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Acid- and Gas-Scavenging Electrolyte Additive Improving the Electrochemical Reversibility of Ni-Rich Cathodes in Li-Ion Batteries
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-04-26 , DOI: 10.1021/acsami.3c02231
Chaeeun Song ₁ , Hyeongyu Moon ₁ , Kyungeun Baek ₂ , Chorong Shin ₃ , Kwansoo Lee ₃ , Seok Ju Kang ₂ , Nam-Soon Choi ₁

Affiliation

In view of their high theoretical capacities, nickel-rich layered oxides are promising cathode materials for high-energy Li-ion batteries. However, the practical applications of these oxides are hindered by transition metal dissolution, microcracking, and gas/reactive compound formation due to the undesired reactions of residual lithium species. Herein, we show that the interfacial degradation of the LiNi_0.9Co_xMn_yAl_zO₂ (NCMA, x + y + z = 0.1) cathode and the graphite (Gr) anode of a representative Li-ion battery by HF can be hindered by supplementing the electrolyte with tert-butyldimethylsilyl glycidyl ether (tBS-GE). The silyl ether moiety of tBS-GE scavenges HF and PF₅, thus stabilizing the interfacial layers on both electrodes, while the epoxide moiety reacts with CO₂ released by the parasitic reaction between HF and Li₂CO₃ on the NCMA surface to afford cyclic carbonates and thus suppresses battery swelling. NCMA/Gr full cells fabricated by supplementing the baseline electrolyte with 0.1 wt % tBS-GE feature an increased capacity retention of 85.5% and deliver a high discharge capacity of 162.9 mAh/g after 500 cycles at 1 C and 25 °C. Thus, our results reveal that the molecular aspect-based design of electrolyte additives can be efficiently used to eliminate reactive species and gas components from Li-ion batteries and increase their performance.

中文翻译：

酸和气体清除电解质添加剂改善锂离子电池中富镍阴极的电化学可逆性

鉴于其高理论容量，富镍层状氧化物是很有前途的高能锂离子电池阴极材料。然而，这些氧化物的实际应用受到过渡金属溶解、微裂纹和由于残留锂物质的不良反应而形成的气体/活性化合物的阻碍。在此，我们表明，典型锂离子电池的LiNi _0.9 Co _x Mn _y Al _z O ₂ (NCMA, x + y + z = 0.1) 阴极和石墨 (Gr) 阳极的界面降解可以是通过用叔补充电解质来阻碍-丁基二甲基甲硅烷基缩水甘油醚 (tBS-GE)。tBS-GE 的甲硅烷基醚部分清除 HF 和 PF ₅，从而稳定两个电极上的界面层，而环氧化物部分与HF 和 Li ₂ CO ₃之间的寄生反应释放的CO _2反应在 NCMA 表面提供环状碳酸酯，从而抑制电池膨胀。通过用 0.1 wt% tBS-GE 补充基线电解质制造的 NCMA/Gr 全电池具有增加的容量保持率 85.5%，并在 1 C 和 25 °C 下循环 500 次后提供 162.9 mAh/g 的高放电容量。因此，我们的研究结果表明，基于分子方面的电解质添加剂设计可以有效地用于消除锂离子电池中的活性物质和气体成分并提高其性能。

更新日期：2023-04-26

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