Design and in situ Characterization of Nanoscale Catalysts

这项拟议的研究涉及利用材料化学合理设计纳米粒子催化剂，用于具有商业意义的氧化和加氢反应。将进行催化剂设计，以提高催化剂的转化率和纳米颗粒催化剂的可回收性，并通过空间隔离催化部位或通过表面功能化控制底物进入纳米颗粒表面来提高催化剂的选择性。此外，纳米颗粒合成和纳米颗粒催化的现场表征将由附近的加拿大光源公司的X射线吸收光谱进行，使用已经开发的用于液体和气相工作的特殊电池。我们在这一领域的长期目标是开发具有高催化活性、对特定底物具有良好的选择性、以及良好的催化剂寿命和回收利用性能的催化剂。因此，我们将开发可持续的催化材料，以最大限度地减少有害物质和溶剂的浪费，并实现昂贵的贵金属催化剂的高原子经济性。*将寻求四个方向，作为设计针对特定应用的纳米粒子催化剂的手段。这些方向包括a)合成用于稳定和选择性加氢和氧化催化剂的硫醇保护的金和双金属簇合物；b)研究纳米颗粒表面催化孤立金属原子位的合成；C)使用离子液体溶剂作为纳米粒子催化的稳定剂和/或助催化剂，以及d)开发一类材料，通过中心等离子体金纳米粒子的光吸收增强催化作用。拟议的研究对加拿大很重要，因为它将使催化剂的设计能够提高石化过程的效率，这是一个具有战略重要性的领域，并将导致培养具有可持续化学和催化过程的纳米材料的合成、表征和应用技能的高素质人员。纳米技术和可持续化学有望为加拿大的石化和材料行业等行业带来巨大利益。**

The proposed research involves the use of materials chemistry for the rational design of nanoparticle catalysts for oxidation and hydrogenation reactions of commercial importance. Catalyst design will be undertaken to improve catalytic turnovers and the recyclability of nanoparticle catalysts, as well as improving catalyst selectivity by spatially isolating catalytic sites or by control of substrate access to nanoparticle surfaces via surface functionalization. In addition, in situ characterization of both nanoparticle synthesis and nanoparticle catalysis will be carried out by X-ray absorption spectroscopy at the nearby Canadian Light Source using specialized cells which have been developed for liquid and gas phase work. Our long-term goal in this field is to develop catalysts which have high catalytic activity, excellent selectivity towards specific substrates, and excellent catalyst longevity and recyclability. Thus we will develop sustainable catalytic materials which can minimize waste of hazardous materials and solvents and attain a high atom economy for expensive noble metal catalysts. ***Four directions will be pursued as a means of designing nanoparticle catalysts directed towards specific applications. These directions include a) the synthesis of thiol-protected gold and bimetallic clusters for stable and selective hydrogenation and oxidation catalysts; b) investigating the synthesis of catalytically isolated metal atom sites on nanoparticle surfaces; c) using ionic liquid solvents as stabilizers and/or cocatalysts for nanoparticle catalysis, and d) the development of a class of materials that allow for the enhancement of catalysis via light absorption by central plasmonic gold nanoparticles.  ***The proposed research is of importance to Canada as it will allow for the design of catalysts which can increase the efficiency of petrochemical processes, an area of strategic importance, and will lead to the generation of highly qualified personnel who have skill-sets in the synthesis, characterization, and applications of nanoscale materials for sustainable chemistry and catalytic processes. Nanotechnology and sustainable chemistry promises to bring tremendous benefits to Canadian sectors such as the petrochemical and materials industry. **