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

本研究的首要目标是了解离子液体（IL，在低温下为液体的盐）和多离子流体中离子键合的性质，以便开发成为普遍接受的合成方法的工具和策略，补充共价键的常规操作以及分子试剂和溶剂的使用。该研究围绕三个主要的科学问题设计，其中独特的离子-离子相互作用和固态化学的结合可以导致新的固态材料或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)为什么锕系元素对软刘易斯碱的亲和力比镧系元素大？ (2)离子液体可以同时作为氧化还原剂、导向剂和脱水剂，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探索通过在低温液态下提供独特的离子环境，在含有f元素的化合物中形成不寻常的化学键的方法。这个问题在研究这些金属在环境中的归宿和迁移或从乏核燃料中分离这些金属时特别重要。目标2的目的是探索离子液体作为反应介质，用于制造固态材料，其中它们巨大的结构多样性允许人们模仿和超过水的反应和溶剂化性质。目的3探索离子液体的可调但完全离子的环境，以获得新的固体形式的药用盐，从而提供对离子相互作用对成核和结晶的影响的基本理解。 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的多离子流体中发现的离子键合，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，采矿和药用盐。基于操纵离子键的化学合成新范式将导致加拿大核、采矿、环境修复和制药工业的重要潜在进步。

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.