Atomic Efficient Catalytic Technology for Sustainable Chemical and Fuel Syntheses Enabled by Active Site Coupling and Kinetic Property Tuning

通过活性位点耦合和动力学特性调节实现可持续化学和燃料合成的原子效率催化技术

• 批准号: RGPIN-2018-06603
• 负责人: Chin, YaHuei(Cathy)
• 金额: $ 8.01万
• 依托单位: University of Toronto
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=747251
• 关键词: Atomic; Efficient; Catalytic; Technology; Sustainable

Efficient synthesis of energy carriers and commodity, specialty, and pharmaceutical chemicals from renewable feedstocks is one of the greatest challenges of this century, paving the path towards a sustainable future. The proposed research program will develop fundamental catalytic knowledge required for this synthesis via the design of catalytic sites and reaction environments and, in turn, tuning of rates and selectivities in order to attain the much sought after atomistic efficiencies. The specific research themes are the conversion of light alkanes, selective hydrogenation of aldehydes/ketones, and coupling of light oxygenates from alternative feedstocks (shale gas, biogas, and lignocellulosic biomass). The program will adapt a highly integrated, multidisciplinary approach, combining advanced spectroscopic and microscopic techniques, density functional theory, together with kinetic and isotopic transient methods, to unravel the catalytic events at the molecular scale. Specific focus is on the structural dynamics of active sites upon their contact with complex solvent mixtures and the instantaneous formation of active structures during catalysis under industrially relevant conditions. Our previous work has established the kinetic functions of well-defined metal and Brønsted acid sites and the catalytic requirements for these reactions with great molecular details. We have also identified key kinetic descriptors, i.e., measurable thermodynamic properties, that dictate the fate of the reactants during their catalytic sojourns. In this next phase, we will exploit the mechanistic knowledge and catalytic requirements, in designing complex, hierarchical catalyst structures with multiple types of mono-functional sites, containing them in confined structures and altering their reaction environment with aggregated solvent molecules for atomic efficient catalysis. Such strategies alter the chemical identity and reactivity of the intermediates and, in turn, dictate the ultimate yields. Incorporating into this program is a comprehensive professional development plan, placing strong emphasis on diverse, interdisciplinary trainings across chemical engineering, chemistry, materials science, as well as on critical thinking and leadership competency. The highly qualified personnel trained from this program will acquire strong technical and professional skill sets with broad industrial and global perspective, through strong, synergistic collaborative efforts and the use of world class infrastructure, within Canada as well as in the US. The personnel will work on fundamental problems, directly transferrable to those in industrial catalysis, as such they are much needed in the Canadian energy and chemical industries.

可再生原料的有效合成能源携带者和商品，专业和药物化学品是本世纪最大的挑战之一，它粘贴了通往可持续未来的道路。拟议的研究计划将通过设计催化位点和反应环境的设计来开发该合成所需的基本催化知识，进而，对速率和选择性进行调整，以便在原子效率之后达到很大的意义。具体的研究主题是轻烷烃的转化，醛/酮的选择性氢化以及来自替代原料（页岩气，沼气和木质纤维素生物量）的光氧偶联的偶联。该程序将适应高度整合的多学科方法，结合高级光谱和微观技术，密度功能理论以及动力学和同位素瞬态方法，以分子尺度揭示催化事件。特定的重点是在活性位点与复杂溶剂混合物接触时的结构动力学以及在工业相关条件下催化过程中有源结构的瞬时形成。我们以前的工作已经建立了定义明确的金属和BrønstedAcid位点的动力学功能，并具有很好的分子细节，对这些反应的催化需求。我们还确定了关键的动力学描述符，即可测量的热力学特性，这些特性决定了反应物在催化静止期间的命运。在下一个阶段，我们将探讨具有多种类型的单功能位点的复合物层次催化剂结构的机械知识和催化需求，其中包含它们在密闭结构中，并用原子效率催化剂的聚集溶剂分子改变其反应环境。中间，反过来决定了最终产量。纳入该计划的是一项全面的专业发展计划，非常重视潜水员，化学工程，化学，材料科学以及批判性思维和领导能力的跨学科培训。经过该计划培训的高素质人员将通过强大的，协同的合作努力以及在加拿大境内以及在美国的世界一流基础设施的使用，并通过广泛的工业和全球视角获得强大的技术和专业技能。这些人员将处理基本问题，直接转移到工业催化的人，因此在加拿大能源和化学工业中急需。