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Mechanistic insight into the improved Li ion conductivity of solid polymer electrolytes

机译:改进固体聚合物电解质的锂离子电导率的机械洞察

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摘要

Polymer based solid electrolytes (SEs) are envisaged as futuristic components of safer solid state energy devices. But the semi-crystalline nature and slow dynamics of the host polymer matrix are found to hamper the ion transport through the solid polymer network and hence solid state devices are still far beyond the scope of practical application. In this study, we unravel the synergistic roles of Li salt (LiClO4) and two different polymers - polyethylene oxide (PEO) and polydimethyl siloxane (PDMS), in the Li ion transport through their solid blend based electrolyte. A detailed study using dielectric spectroscopy and thermo-mechanical analysis is conducted to understand the tunability of the PEO chain dynamics with LiClO4 and the mechanism of hopping of Li ions by forming ion pairs with oxygen dipoles on the PEO backbone is established. Despite the lack of PDMS's capability to solvate ions and promote ion transport directly, its proper mixing within the PEO host matrix is demonstrated to enhance ion transport due to the influence of PDMS on the segmental dynamics of PEO. A detailed molecular dynamics study supported by experimental validation suggests that even inert polymers can affect the dynamics of the active host matrix and increase ion transport, leading to next generation high ionic conductivity solid matrices, and opens new avenues in designing polymer based transparent electrolytes.
机译:基于聚合物的固体电解质(SES)被设想为更安全的固态能量装置的未来派组件。但是,发现主体聚合物基质的半结晶性质和缓慢动力学阻碍了通过固体聚合物网络的离子输送,因此固态装置仍远远超出实际应用的范围。在这项研究中,我们通过其固体共混物基电解质在Li离子输送中解开Li Salt(LiClO4)和两种不同聚合物 - 聚环氧丙烷(PEO)和聚二甲基硅氧烷(PDMS)的协同作用。采用介电光谱和热力学分析的详细研究以了解具有LiCLO4的PEO链动态的可调性,并建立了通​​过在PEO主链上形成离子对,通过在PEO主链上形成离子对的Li离子的跳跃机制。尽管缺乏PDMS对离子的能力并直接促进离子转运,但其在PEO宿主基质内的适当混合被证明是由于PDMS对PEO分段动态的影响,因此引起离子运输。通过实验验证支持的详细分子动力学研究表明,即使是惰性聚合物也会影响活性宿主基质的动态,并增加离子输送,导致下一代高离子电导率固体基质,并在设计基于聚合物的透明电解质时打开新的途径。

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    《RSC Advances》 |2019年第66期|共12页
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  • 正文语种 eng
  • 中图分类 化学;
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