Beyond the age of oxides; new materials for safe and sustainable solid-state batteries.

从手机到客机等应用中最近出现的安全问题突显了高压锂离子电池中液体电解液的潜在危险。如果能够找到一种具有高锂离子导电性和宽潜在工作窗口的综合稳定性(化学和热稳定性)的固体电解质替代品，这种危险是可以避免的。卤化物和氢化物是这一角色的极具吸引力的竞争者，其独特的特点是非氧阴离子可以协同促进锂离子的传输。此外，它们出色的(电)化学稳定性为电池电压超过5V和使用新型、更高活性的阳极(如电极)铺平了道路。该项目涉及设计包含非氧化物多阴离子(例如，硼氢化物、硼烷、复合卤化物)的新材料，在这些材料中，旋转/翻滚的阴离子与高流动性的阳离子在规定的锂离子扩散路径内共生作用。我们的目标是利用这些相互作用(由实验和理论建模)来控制锂离子的迁移率作为阴离子亚晶格的极化率和密度的函数(决定锂离子自由运动的所有方面)。这些概念将被转化为新型固态电池化学，其中Li+被Na+或Mg2+取代作为移动阳离子。这种方法的目的是在不牺牲性能的情况下，迁移到基于更便宜、更丰富的地球金属的更可持续的电池架构。所有新材料都将通过可持续的、节能的方法合成，然后在可充电电池中进行表征和测试。“

"ecent safety issues in applications from cell phones to airliners highlight the potential hazards associated with liquid electrolytes in high voltage Li-ion batteries. Such dangers could be avoided if a solid electrolyte alternative could be found that combined stability (both chemical and thermal) with high Li-ion conductivity and a wide potential operating window. Halides and hydrides are extremely attractive contenders for this role, with the unique feature that the non-oxide anions can promote the transport of Li-cations synergically. Moreover, their outstanding (electro)chemical stability paves the way for cells in excess of 5V and the use of novel, higher activity anodes, such as electrides. This project involves the design of new materials containing non-oxide polyanions (e.g. borohydride, boranes, complex halides) in which rotating/"tumbling" anions interact symbiotically with the highly mobile cations within prescribed Li-ion diffusion pathways. Our ambition is to exploit these interactions (modelled by both experiment and theory) to control the mobility of the Li-ions as a function of the polarisability and density of the anion sublattice (determining all aspects of the free movement of the Li-ions). These concepts will then be translated to novel solid state battery chemistries in which Li+ is replaced by Na+ or Mg2+ as the mobile cation. The aim of this approach is to migrate to more sustainable battery architectures based on cheaper, more Earth-abundant metals, without sacrificing performance. All new materials will be synthesised by sustainable, energy-efficient methods before being characterised and tested in rechargeable cells. "