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.

从可再生原料中高效合成能源载体和商品、特种化学品和医药化学品是本世纪最大的挑战之一，拟议的研究计划将通过设计开发这种合成所需的基础催化知识。具体的研究主题是轻质烷烃的转化、选择性氢化。该项目将采用高度集成的多学科方法，结合先进的光谱和显微技术、密度泛函理论以及动力学和同位素。瞬态方法，以揭示分子尺度的催化事件，特别关注活性位点与复杂溶剂混合物接触和瞬时形成时的结构动力学。我们之前的工作已经建立了明确的金属和布朗斯台德酸位点的动力学函数以及这些反应的催化要求以及大量的分子细节，我们还确定了关键的动力学描述符，即可测量的。热力学性质，决定了反应物在催化停留期间的命运。在下一阶段，我们将利用机械知识和催化要求来设计复杂的分层结构。具有多种类型单功能位点的催化剂结构，将它们包含在有限的结构中，并用聚集的溶剂分子改变其反应环境，以实现原子有效的催化作用，从而改变中间体的化学特性和反应性，进而决定最终的产率。该计划纳入了高度全面的专业发展计划，重点强调化学工程、化学、材料科学等多元化、跨学科的培训以及批判性思维和领导能力，通过该计划培训的合格人员将获得强大的技术。和专业通过加拿大和美国强有力的协同合作和使用世界一流的基础设施，这些人员将致力于解决基本问题，并直接转移到工业催化领域。加拿大能源和化学工业非常需要它们。