Organic salts utilising the hexamethylguanidinium cation: the influence of the anion on the structural, physical and thermal properties†,Physical Chemistry Chemical Physics

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Organic salts utilising the hexamethylguanidinium cation: the influence of the anion on the structural, physical and thermal properties†
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2019-05-29 00:00:00 , DOI: 10.1039/c9cp01740b
Ruhamah Yunis _{1,

2,

3,

4} , Anthony F. Hollenkamp _{4,

5,

6} , Craig Forsyth _{4,

6,

7,

8} , Cara M. Doherty _{4,

6,

9} , Danah Al-Masri _{1,

2,

3,

4} , Jennifer M. Pringle _{1,

2,

3,

4}

Affiliation

The synthesis and characterisation of new solid-state electrolytes is a key step in advancing the development of safer and more reliable electrochemical energy storage technologies. Organic ionic plastic crystals (OIPCs) are an increasingly promising class of material for application in devices such as lithium or sodium metal batteries as they can support high ionic conductivity, with good electrochemical and thermal stability. However, the choice of OIPC-forming ions is still relatively limited. Furthermore, understanding of the influence of different cations and anions on the thermal, structural and transport properties of these materials is still in its infancy. Here we report the synthesis and in-depth characterisation of a range of new OIPCs utilising the hexamethylguanidinium cation ([HMG]) with five different anions. The thermal, structural, transport properties and free volume in the different salts have been investigated. The free volume within the salts has been investigated by positron annihilation lifetime spectroscopy, and the single crystal and powder X-ray diffraction analysis of [HMG] bis(trifluoromethanesulfonyl)imide ([TFSI]) in phase I and II, [HMG] hexafluorophosphate ([PF₆]) and [HMG] tetrafluoroborate ([HMG][BF₄]) are reported. The HMG cation can exhibit significant disorder, which is advantageous for plasticity and future use of these materials as high ionic conductivity matrices. The bis(fluorosulfonyl)imide salt, [HMG][FSI], is identified as particularly promising for use as an electrolyte, with good electrochemical stability and soft mechanical properties. The findings introduce a range of new materials to the solid-state electrolyte arena, while the insights into the physico-chemical relationships in these materials will be of importance for the future development and understanding of other ionic electrolytes.

中文翻译：

利用六甲基胍盐阳离子的有机盐：阴离子对结构，物理和热性能的影响†

新型固态电解质的合成与表征是推动开发更安全，更可靠的电化学储能技术的关键一步。有机离子塑料晶体（OIPC）是一种越来越有前途的材料，可用于锂或钠金属电池等设备，因为它们可以支持高离子电导率，并具有良好的电化学和热稳定性。但是，形成OIPC的离子的选择仍然相对有限。此外，对不同阳离子和阴离子对这些材料的热，结构和传输性能的影响的了解仍处于起步阶段。在这里，我们报告了利用六甲基胍盐阳离子（[HMG]）与五个不同阴离子的一系列新型OIPC的合成和深入表征。散热，结构，已经研究了不同盐中的转运性质和自由体积。已通过正电子an没寿命光谱研究了盐中的自由体积，并对I和II相中的[HMG]双（三氟甲磺酰基）酰亚胺（[TFSI]），[HMG]六氟磷酸盐进行了单晶和粉末X射线衍射分析（[PF_报告了[₆ ]]和[HMG]四氟硼酸盐（[HMG] [BF₄ ]）。HMG阳离子可表现出显着的无序性，这对于可塑性和这些材料作为高离子电导率基质的未来使用是有利的。经鉴定，双（氟磺酰基）酰亚胺盐[HMG] [FSI]具有良好的电化学稳定性和柔软的机械性能，特别有望用作电解质。这些发现为固态电解质领域引入了一系列新材料，而深入了解这些材料中的物理化学关系对于将来开发和理解其他离子电解质将具有重要意义。

更新日期：2019-05-29

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