Do the Ionic Bonds in Ionic Liquids Provide Access to Unique Solid State Chemistry?

这项研究的主要目标是了解离子液体(ILS，低温下为液体的盐)和多离子流体中离子键的性质，以便能够开发出成为普遍接受的合成方法的工具和策略，补充对共价键的传统操作以及分子试剂和溶剂的使用。这项研究围绕三个主要的科学问题进行设计，在这些问题中，独特的离子-离子相互作用和固态化学的结合可以产生新的固态材料，或者可以驱动新的化学反应，并提供关键信息，特别是与核、采矿和制药行业相关的信息。 (1)为什么吖系元素比镧系元素对软Lewis碱有更大的亲和力？ (2)ILS可以同时作为氧化还原、定向和脱水剂，同时也是配体和结晶介质吗？ (3)在离子溶剂中是否可能有独特的多晶型？ 目标1通过在低温下提供独特的液态离子环境，探索在含有f元素的化合物中强制不寻常的化学键的方法。这一问题在研究这些金属在环境中的去向和运输或从乏核燃料中分离这些金属时尤其重要。目标2旨在探索ILS作为制备固态材料的反应介质，其巨大的结构多样性使人能够模仿并超越水的反应和溶解特性。目标3探索离子液体可调节但完全离子的环境，以便能够获得新的固体形式的药物盐，以提供对离子相互作用对成核和结晶的影响的基本了解。 这项研究将利用发现来学习如何设计和控制离子液体和相关多离子流体中的离子键，从而重振研究离子的经典研究领域，如f元素分离、无机材料合成、采矿和药物盐。基于离子键操纵的化学合成的新范例将导致对加拿大的核能、采矿、环境修复和制药工业具有重要意义的潜在进展。

The overarching goal of this research is to understand the nature of ionic bonding in Ionic Liquids (ILs, salts which are liquid at low temperatures) and multi-ion fluids such that tools and strategies can be developed which become generally accepted synthetic methodologies, complementing conventional manipulations of the covalent bond and the use of molecular reagents and solvents. The research is designed around three major scientific questions where the combination of unique ion-ion interactions and solid state chemistry can lead to new solid state materials or can drive new chemical reactions and provide key information, particularly of relevance for the nuclear, mining, and pharma industries. (1) Why do actinides have a greater affinity for soft Lewis bases than lanthanides? (2) Can ILs be simultaneously redox, directing, and dehydrating agents while also being ligands and crystallization media? (3) Are unique polymorphic forms possible in ionic solvents? Objective 1 explores ways to force unusual chemical bonding in compounds containing f-elements by providing unique ionic environments in the liquid state at low temperatures. This question is particularly important in the study of the fate and transport of these metals in the environment or in separations of these metals from spent nuclear fuel. Objective 2 is aimed at exploring ILs as reaction media for making solid state materials, where their tremendous structural diversity allows one to mimic and exceed the reactive and solvating properties of water. Objective 3 explores the tunable yet fully ionic environment of ILs to enable access to new solid forms of pharmaceutical salts to provide fundamental understanding of the effects of ionic interactions on nucleation and crystallization. This research will use discovery to learn how to design and control the ionic bonding found in ILs and related multi-ion fluids and thus reinvigorate classical research areas which study ions, such as f-element separations, inorganic materials synthesis, mining, and pharmaceutical salts. New paradigms for chemical synthesis based on manipulation of ionic bonds will lead to potential advances of importance to Canada’s nuclear, mining, environmental remediation, and pharmaceutical industries.