Next generation catalytic aftertreatment technology for exhaust emission control

减少污染物和温室气体排放是21世纪朝着更清洁的环境和更好的人类健康方向发展的重大挑战。在更广泛的范围内，对具有较强C-H键的未燃烧甲烷等弹性碳氢化合物的催化氧化尤其相关，是一个基本的科学课题，对于开发移动式和固定式发动机排气的创新后处理技术至关重要。目前，北美的甲烷排放在很大程度上仍然不受监管。在未来五年内，新的和即将出台的法规将要求大幅减少汽油/天然气和稀燃(柴油)发动机废气中的甲烷或总碳氢化合物。因此，寻找一种高活性和稳定的催化剂来激活(甲烷中)最强的C-H键的努力已经开始。我们的初步发现表明，具有多层、纳米尺寸、分级的金属-金属氧化物簇合物的C-H键激活的势垒非常低。我们将与三家总部和研发中心位于安大略省的公司(加拿大福特公司、加拿大日立高科技公司和DCL国际公司)合作，以及美国能源部国家实验室和加拿大自然资源部的合作人员，深入研究纳米颗粒的合成和制造，以及使用这些颗粒催化消除顽固碳氢化合物。我们提出了三个主要的研究主题，整合了催化剂的发现和表征、催化途径的基础理解和反应工程，以深入了解催化事件，并制定在大范围燃料与空气操作比下的烃类氧化操作策略。我们采用合成技术、环境电子显微镜和光谱工具，以及动力学、同位素和反应工程方法，来揭开这些催化事件并开发排放控制技术。我们的另一个重点是培训三名博士和一名博士后候选人，他们将直接与我们在安大略省的合作公司合作。

Reducing pollutant and greenhouse gas emissions are the Grand Challenges of 21st century towards a cleaner environment and better human health. Within the broader scope, the catalytic oxidation of resilient hydrocarbons such as unburned methane with strong C-H bonds is especially relevant and a fundamental scientific topic, critical for developing innovative aftertreatment technology for mobile and stationary engine exhausts. Presently, methane emissions remain largely unregulated in North America. Within the next five years, new and upcoming regulations would require significant reduction of methane or the total hydrocarbons in the exhaust streams from gasoline/natural gas and lean burn (diesel) engines. Therefore, the quest to find a highly reactive and stable catalyst for activating the strongest C-H bond (in methane) has begun. Our initial finding has demonstrated the exceptionally low barrier for C-H bond activation with multi-layer, nanometer sized, hierarchical metal-metal oxide clusters. Partnering with three companies (Ford Canada, Hitachi High-Technologies Canada, and DCL International) with headquarters and R&D centres in Ontario, together with collaborators from the U.S. Department of Energy National Lab and Natural Resources Canada, we will investigate in depth the synthesis and fabrication of nanoparticles, the use of these particles for the catalytic abatement of recalcitrant hydrocarbons. We put forward the proposed work with three major research themes, integrating catalyst discovery and characterizations, fundamental understanding of catalytic pathways, and reaction engineering to understand deeply the catalytic events and develop operational strategies for hydrocarbon oxidation under wide ranging fuel-to-air operating ratios. We adapt synthesis techniques, environmental electron microscopic and spectroscopic tools, and kinetic, isotopic, and reaction engineering methods, to unravel these catalytic events and develop the emission control technology. Our other focus is the training of three Ph.D. and one post-doctoral degree candidates, who will work directly with our partnering companies within Ontario.