Towards environmentally friendly processes in materials and energy technologies probed by beta decayed spin spectroscopy and other physical methods

通过β衰变自旋光谱和其他物理方法探索材料和能源技术的环保过程

• 批准号: RGPIN-2014-04194
• 负责人: Ghandi, Khashayar
• 金额: $ 2.24万
• 依托单位: Mount Allison University
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2018
• 资助国家: 加拿大
• 起止时间: 2018-01-01 至 2019-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=651767
• 关键词: Towards; environmentally; friendly; processes; materials

The ultimate goal of this research is to initiate sustainable free radical and radiation-induced processes to develop novel materials with potential applications in technology. The different stages of this research are: *1) microscopic studies with particle-accelerator-based and computational methods; *2) "wet lab" work at Mt. Allison, optimized using our microscopic understanding gained by spectroscopic and theoretical analysis from 1; *3) characterization of the products of the wet lab syntheses with a variety of physical methods, including particle-accelerator based methods if need be (e.g. studies of magnetic or electronic structure properties of the material).*This cycle calls for multifaceted research that will be performed with following foci: *1) free radical and radiation chemistry in green solvents; *2) using sustainable feedstock or waste products of industries or nature to develop value-added materials by free radical and radiation chemistry; and *3) studying the energy efficiency of such processes with or without external fields. *We will minimize the impact of our free radical methods on the environment by finding the most energy-efficient, environmentally friendly solvents. We will experiment with the effects of temperature, pressure, and external fields (such as lasers or microwave (MW)) on free radical reactions to find the most efficient methodology, and to understand the effects of such external fields on the mechanism of free radical reactions. *The novel materials that we plan to make will be: *1) material from free radical reactions in protic ionic liquids dissolved CO2*We have expertise in ionic liquids (ILs), supercritical CO2, high temperature chemistry and reactive free radicals. Therefore a natural extension of our previous studies is to dissolve CO2 in thermally stable ILs then perform free radical reactions on the system. We will focus on modifying our recently synthesized thermally stable protic ILs, but with modified anions (anions with fluorine substitutions have good miscibility with CO2) to polarize CO2, use high temperatures, and free radical precursors to transform CO2 by free radical reactions to commodity chemicals. *These may have potential applications in batteries, fuel cells, components of monomers for ionic polymers for batteries or fuel cells or other applications.*2) Novel nanocomposites based on free radical reactions on the surface of metal or metal oxide nanoparticles. We hope to understand these systems, since free radicals are intermediates in many catalytic processes and for making polymer nanocomposites. *The benefits of these studies will include understanding how to: control or generate new structures on the surface of nanoparticles, tune the electronic and magnetic properties on the surface of nanoparticles, and evaluate the effects of nanoparticles on radiation chemistry. *3) Novel materials based on free radical reactions with enol forms of acids from either biomass or waste products. We will do free radical reactions (e.g. bromination and polymerization) on enol type forms of material in biomass or intermediates in the process of biomass conversion to fuel.*The impacts of our studies are the following: 1) The in situ studies of the effects of MW on free radical reactions have never been done before and we will open the field by our studies. This will help to solve the controversies regarding non thermal effects of MW. 2) Opening the field of in situ free radical transformation of enols in equilibrium with ketones to transform acids (or any compound with C=O or C=N group) from biomass to valuable material. 3) For the first time probing the electronic structures and reactivity of reactive free radicals on the surface of nanoparticles.

这项研究的最终目标是启动可持续的自由基和辐射诱导过程，以开发具有技术潜在应用的新型材料。这项研究的不同阶段是：*1）基于粒子加速器和计算方法的微观研究； *2) Mt. Allison 的“湿实验室”工作，利用我们通过光谱和理论分析从 1 获得的微观理解进行优化； *3) 使用各种物理方法对湿实验室合成产品进行表征，如果需要，包括基于粒子加速器的方法（例如材料的磁性或电子结构特性的研究）。*这个周期需要多方面的研究，将以以下重点进行：*1）绿色溶剂中的自由基和辐射化学； *2）利用可持续原料或工业或自然界的废品，通过自由基和辐射化学开发增值材料； *3) 研究有或没有外部场的此类过程的能源效率。 *我们将通过寻找最节能、最环保的溶剂，最大限度地减少自由基方法对环境的影响。我们将实验温度、压力和外部场（例如激光或微波（MW））对自由基反应的影响，以找到最有效的方法，并了解此类外部场对自由基机理的影响反应。 *我们计划制造的新型材料将是： *1) 质子离子液体溶解 CO2 中自由基反应产生的材料 *我们在离子液体 (IL)、超临界 CO2、高温化学和反应性自由基方面拥有专业知识。因此，我们之前研究的一个自然延伸是将二氧化碳溶解在热稳定的离子液体中，然后在系统上进行自由基反应。我们将专注于修饰我们最近合成的热稳定质子离子液体，但用修饰的阴离子（氟取代的阴离子与CO2具有良好的混溶性）来极化CO2，使用高温和自由基前体通过自由基反应将CO2转化为商品化学品。 *这些可能在电池、燃料电池、电池或燃料电池的离子聚合物单体组分或其他应用中具有潜在应用。*2) 基于金属或金属氧化物纳米颗粒表面自由基反应的新型纳米复合材料。我们希望了解这些系统，因为自由基是许多催化过程和制造聚合物纳米复合材料的中间体。 *这些研究的好处将包括了解如何：控制或生成纳米颗粒表面的新结构，调整纳米颗粒表面的电子和磁性，以及评估纳米颗粒对辐射化学的影响。 *3) 基于与来自生物质或废物的烯醇形式酸的自由基反应的新型材料。我们将对生物质中的烯醇型物质或生物质转化为燃料过程中的中间体进行自由基反应（例如溴化和聚合）。*我们研究的影响如下： 1）影响的原位研究微波对自由基反应的研究以前从未进行过，我们将通过我们的研究打开这个领域。这将有助于解决有关微波非热效应的争议。 2）开辟了烯醇与酮平衡的原位自由基转化领域，以将酸（或任何具有C=O或C=N基团的化合物）从生物质转化为有价值的材料。 3）首次探讨纳米粒子表面活性自由基的电子结构和反应活性。