Powders and Granules in reactive and non-reactive environments

反应性和非反应性环境中的粉末和颗粒

• 批准号: RGPIN-2019-05783
• 负责人: Abatzoglou, Nicolas
• 金额: $ 3.35万
• 依托单位: Université de Sherbrooke
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2020
• 资助国家: 加拿大
• 起止时间: 2020-01-01 至 2021-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=714616
• 关键词: Powders; Granules; reactive; non; environments

The general objective of the proposed research is to study the behaviour of powders and granules in the following contexts: 1. Link nanomorphology of heterogeneous catalysts and more particularly the triple phase boundary length (TPBL) with catalytic activity. The short-term objective and main novelty resides in the adaptation of focused ion beam (FIB) tomography/scanning electron microscopy (SEM) imaging analysis to calculate directly the TPBL and relate it to the catalysts activity. Besides the development of novel catalytic formulations, which could find industrial applications, the main challenge is to develop a protocol allowing for sufficient image contrast and sampling over time-on-stream without affecting catalysts integrity. The methodology relies on the handling of fresh and used formulations and SEM/FIB, transmission electron microscopy (TEM)/electron energy loss spectroscopy (EELS) and TEM/energy dispersive x-ray spectroscopy (EDXS) analyses. Two critical issues is (a) that the catalyst support and catalytic metal containing phases must have significantly different molecular weights to be easily diffentiated by SEM and (b) the choice and use of a resin able to penetrate the open porosity of the catalysts. Once the samples are prepared in accordance with the above, stacks of SEM images are produced from FIB-etched surfaces of the targeted material; each of the so-produced surfaces are SEM micrographed; then, the stack of images are read with an algorithm and the TPBL is estimated from a mathematical 3D reconstruction of the material studied.. 2. Investigate the applicability of a novel patent-pending family of spinel-based nanocatalysts formulated from metallurgical tailings, to catalytic systems requiring optimal metallic phase dispersion. These spinel-based formulations have been proven efficient and robust at various reforming and POX regimes at highretemperature and low pressures. High pressures as well as the use of this catalysts' family to other catalytic reactions are first objective of the proposed research. Three catalytic reactions are targeted: Oxidation, Reduction/Hydrogenation and Alkylation. The methodology is determined by an already advanced literature review and the previous experience of my group and includes the following: functionalization/doping of the UGSO metallurgical residue with the appropriate metal(s); study qualitatively and quantitatively the resulting oxide, spinel and metallic phases and understand the mechanisms of the reactions; relate the nature and the experimental conditions with conversions and selectivity and use them to model the process and propose scale-up criteria. A thermocatalytic scale-up building, equipped with high P and T kg-lab-scale fixed and fluidized bed reactors, is under construction at the Université de Sherbrooke (UdeS), to accommodate my projects, including the ones presented in this proposal and will be available before April 2019.

拟议研究的总体目标是研究粉末和颗粒在以下情况下的行为： 1.将多相催化剂的纳米形态，特别是三相边界长度（TPBL）与催化活性联系起来。短期的目标和主要的新奇在于适应聚焦离子束（FIB）断层扫描/扫描电子显微镜（SEM）成像分析，直接计算TPBL，并将其与催化剂的活性。除了开发可以找到工业应用的新型催化制剂外，主要挑战是开发一种协议，允许在不影响催化剂完整性的情况下随时间推移进行足够的图像对比度和采样。该方法依赖于新鲜和使用过的制剂的处理以及SEM/FIB、透射电子显微镜（TEM）/电子能量损失谱（EELS）和TEM/能量色散X射线光谱（EDXS）分析。两个关键问题是（a）催化剂载体和含催化金属的相必须具有显著不同的分子量以易于通过SEM区分，和（B）选择和使用能够渗透催化剂的开孔孔隙的树脂。一旦根据上述制备样品，就从目标材料的FIB蚀刻表面产生SEM图像的堆叠;对如此产生的表面中的每一个进行SEM显微照相;然后，用算法读取图像的堆叠，并且从所研究的材料的数学3D重建估计TPBL。 2.研究一种由冶金尾矿配制的新型尖晶石基纳米催化剂家族的适用性，该催化剂家族正在申请专利，适用于需要最佳金属相分散的催化系统。这些尖晶石基配方已被证明是有效的和强大的各种重整和POX制度在高温和低压。高压以及将该催化剂家族用于其他催化反应是所提出的研究的第一目标。三个催化反应是目标：氧化，还原/氢化和烷基化。该方法是由一个已经先进的文献综述和以前的经验，我的小组，包括以下内容： 用适当的金属对UGSO冶金残余物进行功能化/掺杂; 定性和定量地研究所产生的氧化物、尖晶石和金属相， 了解反应的机理; 将性质和实验条件与转化率和选择性联系起来，并使用它们来模拟该过程并提出放大标准。 舍布鲁克大学（UdeS）正在建设一个热催化放大建筑，配备高P和T kg实验室规模的固定床和流化床反应器，以适应我的项目，包括本提案中提出的项目，并将于2019年4月之前投入使用。