The development of new ionic electrolytes for energy storage devices Jennifer M. Pringle ,1 Faezeh Makhlooghiazad,1 Azra Sourja,1 Anna Warrington,1 Maria Forsyth1 1Deakin University, 221 Burwood Highway, Burwood, VIC 3125, Australia Electrolytes composed entirely of ions offer important safety and performance advantages over traditional molecular-solvent based systems, particularly for devices utilising reactive metals such as lithium or sodium. The benefits of ionic liquid (IL) based electrolytes are well recognised, while Organic Ionic Plastic Crystals (OIPCs) offer many of the same advantageous features and they are solid at room temperature. An important approach to developing ionic electrolytes that can meet the complex challenges of next-generation electrochemical devices is increasing the range of known and well-characterised salt families. It is recognised that the nature of the cations and anions used to make ionic liquid (IL) electrolytes can have a significant impact on the chemical, physical and electrochemical properties. The same is true for organic ionic plastic crystals (OIPCs); these salts are structurally analogous to ILs and but they are solid at room temperature and display dynamics that can allow their use as solid-state electrolytes.1,2 However, the structure-property relationships are arguably less well understood in OIPCs. Furthermore, the addition of different lithium or sodium salts to these materials, to enable their use in lithium or sodium batteries, introduces further complexities in terms of understanding and optimising the thermal, electrochemical and transport properties. The field of ionic electrolytes can be further expanded by tethering the cation and anion together to form zwitterions. The development of zwitterions with molecular disorder allows their use as the main electrolyte matrix or as additives to polymer electrolytes.3 Here we discuss our development of new plastic crystal-based materials for energy applications, in particular lithium and sodium batteries. We also discuss our recent research into novel zwitterion-based electrolytes. Insights into the relationships between the different ionic and zwitterionic structures and the physical, thermal and electrochemical properties of the resultant electrolytes are presented. References 1. C. S. M. Kang, R. Yunis, H. Zhu, C. M. Doherty, O. E. Hutt and J. M. Pringle Mater. Chem. Front., 2021, 5, 6014-6026 2. A. Warrington, C. S. M. Kang, C. Forsyth, C. M. Doherty, D. Acharya, L. A. O’Dell, N. Sirigiri, J. W. Boyle, O. E. Hutt, M. Forsyth, J. M. Pringle Mater. Chem. Front., 2022, 6, 1437-1455 3. F. Makhlooghiazad, L. A. O’Dell, L. Porcarelli, C. Forsyth, N. Quazi, M. Asadi, O. Hutt, D. Mecerreyes, M. Forsyth, J. M. Pringle, Nat. Mater., 2022, 21, 228
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