CCPR073 - Discovery of inorganic lithium solid electrolytes for all-solid-state batteries

固体电解质（SE）系统的开发是由于开发商业上可行的全固态电池（ASSB）的动机不断增加而不断增长的领域。目前，与ASSB的更高假设能量存储容量相比，人们担心锂离子电池（LIB）技术的局限性。最近，利物浦大学开发了一种新型材料，该材料利用与金属间体系相当的离子排列来产生具有改进的结构多样性和随后的高Li离子导电性的体系（Science，2024，383，739-745）。这样的离子安排有利于广泛的阳离子配位环境，提供低能量障碍和增加离子电导率相比，与其他领先的SE system.The本研究的目的是扩大这种新的结构化学探索新的组合物和材料，可能采用这种结构类型。这涉及阳离子和阴离子物质的多样化。假设进一步增加无序将改善该系统已经令人印象深刻的离子电导率。此外，已知的金属间化合物结构图案和离子导体之间的关系将进一步探索，以确定其他阴离子的安排，是有利的潜在的固态Li离子conductors.In追求扩大这个新系统的能力，该项目将采用计算技术的使用，推导出这个新建立的系统的假设稳定的变化。将采用各种实验方法来寻求实现计算确定的稳定材料，初步的相纯度将通过粉末X射线衍射（PXRD）分析和同步加速器数据来测量。Rietveld精修法将用于确定一种新材料的结构，可能与高分辨率单晶XRD数据相结合。元素分析将随后通过电感耦合等离子体发射光谱（ICP-OES）、CHNS和NMR进行彻底测定。然后，研究将继续量化材料作为固体电解质的性能，通过交流（AC）阻抗测量评估离子电导率，通过直流（DC）极化评估电子电导率。将通过将定量数据和结构分析与从头算分子动力学（AIMD）相结合来理解新开发材料中的Li传输机制，以确定Li传输机制，并有助于全面理解化学空间。

The development of solid electrolyte (SE) systems is a field that is ever-growing due to the increasing motivation to develop a commercially viable all-solid-state battery (ASSB). Currently, there are concerns with the limitations of Li-ion battery (LIB) technology, when compared with the higher hypothetical energy storage capacity of ASSBs. A focal point of ASSB development is the advancement of the state-of-the-art of solid electrolytes.Recently, a novel material was developed at the University of Liverpool, that utilised ion arrangements comparable to intermetallic systems to produce a system that has improved structural diversity and subsequently a high Li ion conductivity (Science, 2024, 383, 739-745). Such ion arrangements facilitate a wide array of cation coordination environments, providing low energy barriers and increased ionic conductivity when compared with other leading SE systems.The purpose of this research is to expand on this new structural chemistry by exploring new compositions and materials that may adopt this structure type. This involves diversification of cationic and anionic species. The hypothesis being that further increased disorder will improve the already impressive ionic conductivity of this system. Additionally, the relationship between known intermetallic structural motifs and ionic conductors will be explored further to identify other anion arrangements that are favourable as potential solid state Li ion conductors.In the pursuit to expand the capability of this novel system, the project will employ the use of computational techniques to derive hypothetically stable variations of this newly established system. Varied experimental approaches will be employed to seek to achieve computationally determined stable materials, with preliminary phase purity will be measured by Powder X-Ray Diffraction (PXRD) analysis and synchrotron data. Rietveld refinement will be used to characterise the structure of a novel material, possibly in combination with high-resolution single crystal XRD data.Elemental analysis will be thoroughly determined thereafter by inductively coupled plasma optical emission spectroscopy (ICP-OES), CHNS and NMR. Studies will then go on to quantify the performance of the material as a solid electrolyte, assessing the ionic conductivity by alternating current (AC) impedance measurements and electronic conductivity by direct current (DC) polarization. The Li-transport mechanism in newly developed materials will be understood by combining quantitative data and structural analysis with ab initio molecular dynamics (AIMD) to determine the Li transport mechanism and contribute overall to the understanding of the chemical space.