How to Harvest Grotthuss Diffusion in Protic Ionic Liquid Electrolyte Systems,ChemSusChem

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How to Harvest Grotthuss Diffusion in Protic Ionic Liquid Electrolyte Systems
ChemSusChem ( IF 7.5 ) Pub Date : 2018-06-15 , DOI: 10.1002/cssc.201800436
Johannes Ingenmey ₁ , Sascha Gehrke _{1,

2} , Barbara Kirchner ₁

Affiliation

Hydrogen is often regarded as fuel of the future, and there is an increasing demand for the development of anhydrous proton‐conducting electrolytes to enable fuel‐cell operation at elevated temperatures exceeding 120 °C. Much attention has been directed at protic ionic liquids as promising candidates, but in the search for highly conductive systems the possibility of designing Grotthuss diffusion‐enabled protic ionic liquids has been widely overlooked. Herein, the mechanics of proton‐transfer mechanism in the equimolar mixture of N‐methylimidazole and acetic acid was explored using ab initio molecular dynamics simulations. The ionicity of the system is approximated with good agreement to experiments. This system consists mostly of neutral species but exhibits a high ionic conductivity through Grotthuss‐like proton conduction. Chains of acetic‐acid molecules and other species participating in the proton‐transfer mechanisms resembling Grotthuss diffusion could be directly observed. Furthermore, based on these findings, a series of static quantum chemical calculations was conducted to investigate the effect of substituting the anion and cation with different functional groups. We predict whether a given combination of cation and anion will be a true ionic liquid or a molecular mixture and propose some systems as candidates for Grotthuss diffusion‐enabled protic ionic liquids.

中文翻译：

如何在质子离子液体电解质系统中收获格罗特斯扩散

氢通常被认为是未来的燃料，对开发无水质子传导电解质的需求不断增长，以使燃料电池能够在超过120°C的高温下运行。质子离子液体已成为备受关注的候选物，引起了很多关注，但是在寻找高导电性系统时，设计Grotthuss能够扩散扩散的质子离子液体的可能性已被广泛忽略。在这里，氮等摩尔混合物中质子转移机理的力学使用从头开始的分子动力学模拟对甲基咪唑和乙酸进行了研究。该系统的电离度与实验吻合良好。该系统主要由中性物质组成，但通过格罗索斯样质子传导表现出高离子电导率。可以直接观察到醋酸分子分子链和其他类似质子扩散的质子转移机制。此外，基于这些发现，进行了一系列静态量子化学计算，以研究用不同官能团取代阴离子和阳离子的效果。我们预测给定的阳离子和阴离子组合将是真正的离子液体还是分子混合物，并提出了一些系统作为Grotthuss能够扩散的质子离子液体的候选对象。

更新日期：2018-06-15

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