Design and in situ Characterization of High-Surface Area Metallic and Bimetallic Nanoscale Catalysts

建议的研究涉及使用材料化学来合理设计用于选择性氧化和加氢反应的纳米催化剂。将进行催化剂设计，以提高纳米颗粒催化剂的活性和稳定性，并通过空间隔离催化部位或通过控制底物访问纳米颗粒表面来提高催化剂的选择性。此外，纳米颗粒设计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，以最大限度地减少危险材料和溶剂的浪费，并实现昂贵的贵金属催化剂的高原子经济性。 具体地说，将寻求三个方向作为设计针对特定应用的纳米颗粒催化剂的手段。这些方向包括a)合成原子精确的金属和双金属簇合物，用于稳定和选择性的加氢和氧化催化剂；b)催化金属在金属氧化物纳米颗粒载体上的电偶还原，以及c)通过纳米颗粒的脱合金化和利用这种纳米颗粒的内腔来加速催化反应来合成和表征多孔纳米颗粒催化剂。 拟议的研究对加拿大很重要，因为它将允许设计能够提高石化过程效率的催化剂，并将产生具有可持续化学和催化过程中纳米材料的合成、表征和应用技能的HQP。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 toward the rational design of nanoparticle catalysts for selective oxidation and hydrogenation reactions. Catalyst design will be undertaken to improve activity and stability of nanoparticle catalysts, as well as improving catalyst selectivity by spatially isolating catalytic sites or by control of substrate access to nanoparticle surfaces. In addition, in situ characterization of both nanoparticle design 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 be developing sustainable catalytic materials which can minimize waste of hazardous materials and solvents, and attain a high atom economy for expensive noble metal catalysts. Specifically three directions will be pursued as a means of designing nanoparticle catalysts directed towards specific applications. These directions include a) the synthesis of atom-precise metallic and bimetallic clusters for stable and selective hydrogenation and oxidation catalysts; b) galvanic reductions of catalytic metals onto metal oxide nanoparticle supports, and c) the synthesis and characterization of porous nanoparticle catalysts via dealloying of nanoparticles and using the interior cavities of such nanoparticles to accelerate catalytic reactions. 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 and will lead to the generation of HQP 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.