Electrochemical dynamics of nanoparticles suspended in an ionic liquid or organic ionic plastic crystal

我们研究计划的主要目标是开发用于健康、储能和催化应用的多功能、柔性/可模塑电极和电解液材料。长期目标将是评估将塑料块体材料性能与嵌入的金属纳米颗粒(NPs)结合在一起的纳米复合材料，以提高反应性以及改善离子和电子传导性。由于电极反应是非均相的，发生在固-溶液或不相容的液-液界面上，了解界面反应机理和动力学/热力学对于优化电极材料的性能至关重要。这是复杂的表面形态(例如粗糙度)，它抑制或加强物种的吸附。对于去卷曲的界面反应，我们将使用高分辨率(纳米级)电化学成像，它同时在原位和在操作区成像表面的电活性和形貌。这些纳米探针能够区分单个NPs。物理化学和电催化信息反过来又是设备性能的直接衡量标准。通过这种方式，我们将评估材料的适宜性，并填补基础物理化学知识的空白。结合传统的电化学方法(如循环伏安法和阻抗谱)，我们将开发纳米复合材料性能的预测模型，这将使我们能够开发新的技术和新的扫描探针方法。我们还将在我们的纳米探测器中安装电活性材料，以制造高灵敏度的概念验证(BIO)传感器。对于悬浮在液体介质中的NPs，我们将使用单个NP跟踪和随机NP撞击检测等技术来阐明NP的反应性和NP的产生/销毁过程。短期目标将集中在离子液体(ILS)或有机离子塑料晶体(OIPC)中嵌入的金属纳米颗粒。ILS在室温下是液体，而OIPC是塑料。通过我们的扫描探针方法，我们将深入了解NP-NP和NP-IL/NP-OIPC的相互作用。我们将探索简单的一步电荷转移过程，直到多步电催化。还将研究NPs对IL和OIPC薄膜的物理化学和形态特性的影响，在这些薄膜中，它们分别被证明可以提高粘度和缺陷/晶界的形成。这些反过来又增强了离子和电子的传导性。纳米粒子在OIPC的电催化中的作用几乎是未知的，将是纪念馆研究小组的一个主要重点。我们的工作将有助于加拿大在电催化、先进传感、能量储存/收集、高分辨率扫描探针成像和光学光谱学领域的领先地位。HQP将开发高度重视的电分析、扫描探针、计算、合成和材料表征技能。

The main objective of our research program is the development of multi-purpose, flexible/mouldable electrode and electrolyte materials for health, energy storage, and catalytic applications. Long-term objectives will be towards evaluating nanocomposite materials incorporating plastic bulk material properties with embedded metal nanoparticles (NPs) for enhanced reactivity as well as improved ionic and electronic conductivity. Since electrode reactions are heterogeneous, occurring at either solid|solution or immiscible liquid|liquid interfaces, understanding interfacial reaction mechanisms and kinetics/thermodynamics is crucial for optimizing electrode material performance. This is complicated by the surface morphology (e.g. roughness),  which inhibit or enhance species adsorption. To deconvolute interfacial reactions, we will use high-resolution (nanoscale) electrochemical imaging, which images surface electroactivity and topography, simultaneously in situ and in operando. These nanoprobes are capable of distinguishing single NPs. Physicochemical and electrocatalytic information is in turn a direct measure of device performance. In this way, we will assess material suitability and fill gaps in fundamental physical/material chemistry knowledge. Combined with conventional electrochemical methods (e.g. cyclic voltammetry and impedance spectroscopy), we will develop predictive models of nanocomposite material performance, which will enable us to develop new technologies and new scanning probe methodologies. We will also install electroactive materials into our nanoprobes to make highly sensitive proof-of-concept (bio)sensors. For NPs suspended in liquid media, we will employ techniques such as single NP tracking in tandem with stochastic NP impact detection to elucidate NP reactivity and NP generation/destruction processes. Short-term objectives will focus on metal NPs embedded in ionic liquids (ILs) or organic ionic plastic crystals (OIPCs). ILs are liquid at room temperature, while OIPCs are plastic. Through our scanning probe methods, we will gain insight into NP-NP and NP-IL/NP-OIPC interactions. We will explore simple one-step charge transfer processes, up to multi-step electrocatalysis. The impact of NPs on the physicochemical and morphological properties of IL and OIPC films will also be investigated, where they have been shown to enhance viscosity and the formation of defects/grain boundaries, respectively. These in-turn enhance ionic and electronic conductivity. The role of NPs in electrocatalysis in OIPC is virtually unexplored and will be a major focus of the research team at Memorial. Our work will contribute to Canada's leadership in the fields of electrocatalysis, advanced sensing, energy storage/harvesting, high resolution scanning probe imaging, and optical spectroscopy. HQP will develop highly valued electroanalytical, scanning probe, computational, synthetic, and materials characterization skills.