CAREER: CAS: Understanding How Catalyst Modification Impacts Performance Thermodynamic and Kinetic Parameters Pertinent to Catalytic Hydrogenation of Polar Carbonyl Bonds

职业：CAS：了解催化剂改性如何影响与极性羰基键催化氢化相关的性能热力学和动力学参数

• 批准号: 1945646
• 负责人: Caroline Saouma
• 金额: $ 67.5万
• 依托单位: University of Utah
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-04-01 至 2025-03-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1945646&HistoricalAwards=false
• 关键词: CAREER; CAS; Understanding; How; Catalyst

To meet our future energy needs, new chemical reactions that use carbon dioxide (CO2) and other waste products to produce fuels and chemical feedstocks need to be developed. The use of CO2 as a starting material is challenging because it is a gas and not very reactive. Scientists like Dr. Saouma at the University of Utah develop cheap and readily-available catalysts to speed up these reactions. This research project focuses on developing an understanding of how catalyst structure impacts the catalyst performance. This knowledge allows more efficient and effective better catalysts to be prepared. Dr. Saouma is actively engaged in outreach activities that aim to increase female representation in Science, Technology, Engineering, and Math (STEM) fields. She is an instructor and mentor for the College of Science’s ACCESS program, an intensive summer-long program for incoming freshman women that provides them with a comprehensive view of how energy is produced and used in our society. A survey of high school seniors in Utah indicates that prior to college a gender gap exists in students interested in STEM fields. To help offset this, Dr. Saouma is developing an offshoot of ACCESS that is geared towards increasing the number of rising ninth grade women. participating in science.With funding from the Chemical Structure, Dynamics and Mechanisms-B and the Chemical Catalysis Programs of the Chemistry Division, Dr. Saouma of the University of Utah is developing a fundamental understanding that correlates the thermodynamic properties of a catalyst with catalyst performance for systems that reduce carbonyl bonds. The research measures how ligand and metal identities impact parameters such as hydricity and propensity to add H2 in systems that undergo metal ligand cooperativity and these characteristics are compared through equilibrium measurements. These measurements are also correlated to the catalyst performance in terms of kinetics, mechanism, and scope. Parallel work on developing ligands that are designed to allow separate tuning of the thermodynamic parameters is also under investigation. Dr. Saouma is part of the College of Science’s ACCESS program, whose mission is to increase the representation of women in leadership in the STEM disciplines. In addition to mentoring and instructing the incoming freshman women of ACCESS, Dr. Saouma is developing a sister program that will encompass a summer camp for rising 9th graders, to help address the gender discrepancy in STEM interest that exists amongst high school students in Utah.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

为了满足我们未来的能源需求，需要开发新的化学反应，利用二氧化碳(CO2)和其他废物来生产燃料和化学原料。使用二氧化碳作为起始材料是具有挑战性的，因为它是一种气体，活性不是很强。像犹他大学的索玛博士这样的科学家开发了廉价且容易获得的催化剂来加速这些反应。本研究项目致力于加深对催化剂结构如何影响催化剂性能的理解。这一知识使得制备更高效、更有效的催化剂成为可能。Saouma博士积极参与旨在增加女性在科学、技术、工程和数学(STEM)领域的代表性的外联活动。她是科学学院Access计划的讲师和导师，这是一个为新生女性提供的为期一年的暑期强化计划，让她们全面了解能源在我们的社会中是如何生产和使用的。一项针对犹他州高三学生的调查显示，在大学之前，对STEM领域感兴趣的学生中存在性别差异。为了帮助抵消这一影响，佐玛博士正在开发Access的一个分支，旨在增加正在上九年级的女性人数。在化学结构、动力学和机理-B以及化学系化学催化计划的资助下，犹他大学的Saouma博士正在发展一种基本的理解，即将催化剂的热力学性质与还原羰基的体系的催化剂性能相关联。这项研究测量了配体和金属的同一性如何影响经历金属配体协同作用的体系中的参数，如氢化度和加氢倾向，并通过平衡测量比较了这些特征。这些测量也与催化剂的性能在动力学、机理和范围方面相关联。开发配体的平行工作也在调查中，这些配体旨在允许单独调整热力学参数。Saouma博士是科学学院Access计划的一部分，该计划的使命是增加女性在STEM学科中的领导地位。除了指导和指导即将入学的新生女性，Saouma博士正在开发一个姊妹项目，其中将包括为9年级高年级学生举办的夏令营，以帮助解决犹他州高中生在STEM兴趣方面存在的性别差异。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Ru catalyzed hydrogenation of CO2 to formate under basic and acidic conditions

• DOI: 10.1016/j.poly.2021.115375
• 发表时间: 2021-07
• 期刊: Polyhedron
• 影响因子: 2.6
• 作者: Austin T Cannon;C. Saouma

Large changes in hydricity as a function of charge and not metal in (PNP)M–H (de)hydrogenation catalysts that undergo metal–ligand cooperativity

• DOI: 10.1039/d2cy01349e
• 发表时间: 2023
• 期刊: Catalysis Science & Technology
• 作者: Kevin Schlenker;Lillee K. Casselman;R. Vanderlinden;C. Saouma

Correction to “Thermodynamic Analysis of Metal–Ligand Cooperativity of PNP Ru Complexes: Implications for CO 2 Hydrogenation to Methanol and Catalyst Inhibition”

对“金属热力学分析”PNP Ru 配合物的配体协同性的修正：对 CO 2 加氢生成甲醇和催化剂抑制的影响

• DOI: 10.1021/jacs.1c06789
• 发表时间: 2021
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Mathis, Cheryl L.;Geary, Jackson;Ardon, Yotam;Reese, Maxwell S.;Philliber, Mallory A.;VanderLinden, Ryan T.;Saouma, Caroline T.
• 通讯作者: Saouma, Caroline T.