Solid-State NMR Revealing the Impact of Polymer Additives on Li-Ion Motions in Plastic-Crystalline Succinonitrile Electrolytes,The Journal of Physical Chemistry C

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Solid-State NMR Revealing the Impact of Polymer Additives on Li-Ion Motions in Plastic-Crystalline Succinonitrile Electrolytes
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2023-01-10 , DOI: 10.1021/acs.jpcc.2c05526
Julia Möller ₁ , Vanessa van Laack ₂ , Katharina Koschek ₂ , Patrick Bottke ₁ , Michael Wark ₁

Affiliation

To enhance the safety of lithium-ion batteries (LIBs), alternatives to liquid electrolytes are widely studied. One of them is the plastic-crystal succinonitrile (SN) which is able to solvate various Li salts. This system can be further extended by inserting polymers, bringing additional advantages such as higher melting points and the possibility of adjusting thermo-mechanical and electrochemical properties. The plastic-crystalline electrolyte consisting of the Li salt lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) dissolved in SN was extended by adding various thermoplastic polymers, namely, polyacrylonitrile (PAN), poly(ethylene oxide) (PEO), polyethylene carbonate (PEC), and polyvinylpyrrolidone (PVP). Even small amounts (10 wt %) of added polymer to the SN-base were found to impact the Li-ion mobility. Variable temperature investigations on structure and ion dynamics were performed using static and magic angle spinning (MAS) solid-state NMR and various relaxometry measurements. Influence of the Li concentration and the polymers’ functional groups on the structure of SN and the resulting Li-ion mobility was elaborated. Activation energies and jump rates of the Li ions were determined. As a result, the PAN-containing system stands out to be a promising candidate for application in future LIBs as it shows high ion mobility, low activation energy, and a high potential for further modifications. Solid-state NMR turned out to be a reliable method and a good alternative to impedance spectroscopy measurements for investigating ion mobility behavior providing even more information.

中文翻译：

固态核磁共振揭示了聚合物添加剂对塑晶丁二腈电解质中锂离子运动的影响

为了提高锂离子电池 (LIB) 的安全性，人们广泛研究了液体电解质的替代品。其中之一是塑晶丁二腈 (SN)，它能够溶剂化各种锂盐。该系统可以通过插入聚合物进一步扩展，带来额外的优势，例如更高的熔点以及调整热机械和电化学性能的可能性。通过添加各种热塑性聚合物，即聚丙烯腈（PAN）、聚（环氧乙烷）（PEO）、聚碳酸亚乙酯（PEC），扩展了由溶解在 SN 中的锂盐双（三氟甲磺酰基）亚胺锂（LiTFSI）组成的塑性结晶电解质) 和聚乙烯吡咯烷酮 (PVP)。发现即使少量（10 wt%）添加到 SN 基中的聚合物也会影响锂离子迁移率。使用静态和魔角旋转 (MAS) 固态核磁共振和各种弛豫测量对结构和离子动力学进行变温研究。阐述了 Li 浓度和聚合物官能团对 SN 结构和由此产生的锂离子迁移率的影响。测定了锂离子的活化能和跳跃率。因此，含 PAN 的系统脱颖而出，成为未来 LIB 应用的有希望的候选者，因为它显示出高离子迁移率、低活化能和进一步修饰的高潜力。事实证明，固态核磁共振是一种可靠的方法，也是阻抗谱测量的良好替代方法，可用于研究离子淌度行为，提供更多信息。

更新日期：2023-01-10

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