Catalysis for Green Fuel Processes and Environmental Remediation

气候变化是当今社会面临的一个巨大挑战，虽然向电动和混合动力汽车的转变进展缓慢，但内燃机使用的燃料需要更环保的替代品。这在加拿大尤其重要，因为在加拿大，使用电动车辆可能不适用于农业、内陆运输、海洋运输或农村或孤立的北部土著社区。最近的绿色燃料趋势包括生物质发酵生产乙醇作为生物燃料，以及通过电催化过程将二氧化碳还原为甲醇。甲醇和乙醇都是绿色火花点火（SI）发动机的候选燃料，但在压缩点火（CI）发动机应用中需要升级。甲醇和乙醇可分别升级为二甲醚和乙醚。在我的研究计划中，我的目标是研究从二氧化碳中生产二甲醚的反应网络，并确定可能的催化过程，使这些燃料的生产在工业上可行，并在加拿大广泛使用。在生产这些二甲醚和乙醚燃料时，必须确保使用这些燃料产生的排放符合环境法规，这是我研究计划的第二个目标。总而言之，这个研究项目的目标是围绕以化学和催化为中心的绿色和替代燃料的生产设计可持续的过程。我们将使用过程建模和分析来确定从二氧化碳到二甲醚的最佳反应途径。这个过程分析将帮助我们确定我们想要如何耦合反应，我们有什么机会通过耦合反应来克服反应过程中的热力学限制，以及最终催化剂需要在什么标准和操作条件下运行。在机制层面上理解反应将导致在过程层面上的见解，这就是为什么我们将进行仔细的动力学和力学研究来创建和验证动力学模型。我们还将整合双功能催化剂上偶联反应的思想和/或合理设计专门为这些新型催化过程设计的催化剂结构。为了使CI或SI发动机的绿色燃料排放符合环保法规，我们将合理设计排放催化剂，氧化未燃烧的碳氢化合物和一氧化碳，减少使用这些燃料或燃料混合物的发动机技术排放的氮氧化物。我们可以通过动力学和力学研究来测试和改进我们的催化剂设计。

Climate change is a grand challenge facing society today, and while the move to electric and hybrid vehicles is happening slowly, there needs to be greener alternatives available for fuels used in internal combustion engines. This is particularly relevant in Canada, where the use of electrified vehicles may not be practical for the agricultural industry, for moving freight inland, for marine transport, or for rural or isolated northern indigenous communities. Recent green fuel trends include the fermentation of biomass to produce ethanol as a biofuel, and the reduction of carbon dioxide to methanol via electrocatalytic processes. Methanol and ethanol are both candidates for green spark ignition (SI) engine fuels, however need upgrading for use in compression ignition (CI) engine applications. Methanol and ethanol can be upgraded to dimethyl ether and diethyl ether respectively. In my research program, my objective is to investigate the reaction networks for the production of dimethyl ether from carbon dioxide and identify possible catalytic processes that will make the production of these fuels industrially feasible, and attractive for widespread use across Canada. With the production of these dimethyl ether and diethyl ether fuels, it must be ensured that the emissions from using these as fuels meet environmental regulations, which constitutes the second objective of my research program. To summarize, the goal of this research program is to design sustainable processes around producing green and alternative fuels centered around the chemistry and catalysis. We will use process modeling and analysis to determine the best reaction pathway from carbon dioxide to dimethyl ether. This process analysis will help us determine how we want to couple reactions, what opportunities we have to overcome any thermodynamic limitations during reactions by coupling reactions, and ultimately what criteria and operating conditions the catalyst will need to operate under. Understanding reactions at the mechanistic level will lead to insights at the process level, which is why we will perform careful kinetic and mechanistic studies to create and validate kinetic models. We will also integrate the ideas of coupling reactions over dual functional catalysts and/or rationally designing catalyst architectures which are specially designed for these novel catalytic processes. For the emissions of green fuels in CI or SI engines to meet environmental regulations, we will rationally design the emissions catalysts to oxidize the unburnt hydrocarbons and carbon monoxide and reduce nitrogen oxides for the emissions for engine technologies using these fuels or fuel blends. We can test and then refine our catalyst design through kinetic and mechanistic studies.