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: 2019
• 资助国家: 加拿大
• 起止时间: 2019-01-01 至 2020-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=689351
• 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在以下背景下研究粉末和颗粒的行为：*1.非均相催化剂的纳米形态，尤其是三相界面长度(TPBL)与催化活性的联系。短期目标和主要创新在于采用聚焦离子束(FIB)层析/扫描电子显微镜(SEM)成像分析来直接计算TPBL并将其与催化剂活性相关联。除了开发可用于工业应用的新型催化配方外，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，随着时间的推移实现足够的图像对比度和采样。该方法依赖于新鲜和二手配方的处理以及扫描电子显微镜/FIB、透射电子显微镜(TEM)/电子能量损失谱(EELS)和透射电子显微镜/能量色散X射线光谱(EDXS)分析。两个关键问题是(A)催化剂载体和催化金属相必须具有明显不同的分子质量，以便通过扫描电子显微镜进行区分；(B)能够穿透催化剂开口孔洞的树脂的选择和使用。一旦按照上述方法制备样品，从目标材料的FIB蚀刻表面产生层叠的扫描电子显微镜图像；对每个如此产生的表面进行扫描电子显微镜显微成像；然后，用算法读取该层叠图像，并根据所研究材料的数学3D重建来估计TPBL。*2.研究由冶金尾矿配制的新型尖晶石基纳米催化剂家族正在申请专利，对需要最佳金属相分散的催化系统的适用性。事实证明，这些基于尖晶石的配方在高温和低压下的各种重整和POX制度下都是有效和坚固的。高压以及将这种催化剂家族用于其他催化反应是拟议研究的首要目标。有三个催化反应：氧化、还原/氢化和烷基化。该方法是根据已经很先进的文献综述和本小组以前的经验确定的，包括以下内容：*用适当的金属对UGSO冶金残渣进行官能化/掺杂(S)；*对生成的氧化物、尖晶石和金属相进行定性和定量研究，并*了解反应机理；*将性质和实验条件与转化率和选择性联系起来，并使用它们来模拟过程并提出放大标准。*正在舍布鲁克大学(UDES)建造一座热催化放大建筑，配备高P和T公斤实验室规模的固定床和沸腾床反应器，以容纳我的项目，包括本提案中提出的项目，将于2019年4月之前交付使用。