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，需要开发利用二氧化碳 (CO2) 和其他废物生产燃料和化学原料的新化学反应。使用二氧化碳作为起始材料具有挑战性，因为它是一种气体，而且性质不太好。犹他大学的 Saouma 博士等科学家开发了廉价且易于使用的催化剂来加速这些反应，该研究项目的重点是了解催化剂结构如何影响催化剂性能。催化剂成为Saouma 博士积极参与旨在提高科学、技术、工程和数学 (STEM) 领域女性代表性的外展活动。她是理学院 ACCESS 项目（夏季强化项目）的讲师和导师。一项针对犹他州高中生的调查表明，在大学之前对 STEM 领域感兴趣的学生中存在性别差距。 Saouma 博士是这样的开发 ACCESS 的一个分支，旨在增加九年级女性参与科学的人数。在化学结构、动力学和机制-B 以及化学系化学催化项目的资助下，Saouma 博士获得了该项目的资助。犹他州正在开发一种基本的理解，将催化剂的热力学性质与减少羰基键的系统的催化剂性能联系起来。该研究测量了配体和金属特性如何影响参数，例如水硬性和添加 H2 的倾向。在经历金属配体协同作用的系统中，这些特征通过平衡测量进行比较，这些测量也与动力学、机制和范围方面的催化剂性能相关。 Saouma 博士是理学院 ACCESS 计划的一部分，该计划的任务是除了指导和指导即将入学的女性新生外，还提高女性在 STEM 学科领导层中的代表性。 ACCESS，Saouma 博士正在开发一个姐妹项目，其中包括为 9 年级新生举办夏令营，以帮助解决犹他州高中生对 STEM 兴趣存在的性别差异。该奖项反映了 NSF 的法定使命，并被认为是值得的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来获得支持。

项目成果

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

Ru在碱性和酸性条件下催化CO2加氢生成甲酸盐

• DOI: 10.1016/j.poly.2021.115375
• 发表时间: 2021-07-21
• 期刊: Polyhedron
• 影响因子: 2.6
• 作者: Austin T Cannon;C. Saouma
• 通讯作者: 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

在经历金属-配体协同作用的 (PNP)M–H（脱）加氢催化剂中，氢度随电荷而非金属发生巨大变化

• DOI: 10.1039/d2cy01349e
• 发表时间: 2024-09-14
• 期刊: Catalysis Science & Technology
• 作者: Kevin Schlenker;Lillee K. Casselman;R. V;erlinden;erlinden;C. Saouma
• 通讯作者: C. Saouma

Role of Ligand-Bound CO 2 in the Hydrogenation of CO 2 to Formate with a (PNP)Mn Catalyst

配体结合的 CO 2 在 (PNP)Mn 催化剂的 CO 2 加氢生成甲酸盐中的作用

• DOI: 10.1021/acscatal.1c01709
• 发表时间: 2021-07
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Schlenker, Kevin;Christensen, Elizabeth G.;Zhanserkeev, Asylbek A.;McDonald, Gabriel R.;Yang, Emily L.;Lutz, Kevin T.;Steele, Ryan P.;VanderLinden, Ryan T.;Saouma, Caroline T.
• 通讯作者: Saouma, Caroline T.

Hydrogenation and electrocatalytic reduction of carbon dioxide to formate with a single Co catalyst

使用单一 Co 催化剂氢化和电催化还原二氧化碳生成甲酸盐

• DOI: 10.1039/d0cc04310a
• 发表时间: 2020-10
• 期刊: Chemical Communications
• 影响因子: 4.9
• 作者: Wang, Fang;Cannon, Austin T.;Bhattacharya, Moumita;Baumgarten, Robert;VanderLinden, Ryan T.;Saouma, Caroline T.
• 通讯作者: Saouma, Caroline T.

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: 2021-07
• 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.