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Enabling Redox Reactions for Catalysis with Group 13 Elements

使用第 13 族元素实现催化氧化还原反应

基本信息

批准号：
1763821
负责人：
Louise Berben
金额：
$ 45.7万
依托单位：
University of California-Davis
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-09-01 至 2023-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1763821&HistoricalAwards=false
关键词：
Enabling Redox Reactions Catalysis Group

项目摘要

With funding from the Chemical Synthesis program of the Division of Chemistry, Dr. Louise Berben of the University of California-Davis is studying the reaction chemistry of the sustainable element aluminum. This work provides needed insight into environmentally-friendly industrial processes and advanced manufacturing. Dr. Berben is generating knowledge that can be applied broadly in both heterogeneous (i.e., solid state) and homogeneous (i.e., in solution) catalysis. This project contributes to the creation of an environmentally- and economically-sustainable chemical industry, and to the efficient conversion of feedstocks to value-added chemicals. Other impacts are in preparing a workforce of skilled synthetic inorganic chemists specializing in main group elements, which is needed for the creation of modern materials and electronics, and in sustainable approaches to large scale chemical synthesis. Dr. Berben is also partnering with national programs to mentor economically-disadvantaged high school students and undergraduates in research projects. These outreach efforts are interwoven with her scientific contributions. Dr. Berben is exploring molecular redox-active ligand complexes of aluminum (Al) and gallium (Ga) to understand mechanisms of proton and electron transfer to generate hydride equivalents, thereby establishing correlations between molecular structure, thermochemistry, and reactivity of hydride transfer reactions. Dr. Berben is also exploring redox-mediated substrate activation pathways for these reactions. Specific areas of investigation include the synthesis of new ligands and metal-ligand molecules that mediate generation of hydride equivalents via ligand-based proton and electron transfer chemistry. The research group characterizes metal-ligand complex via pKa and hydricity values as well as hydride transfer reactivity, so that structure-property-reactivity correlations can be established. These characterization studies inform the choice of reaction conditions and new molecular design. Building on the redox-active Group 13 molecules that are being developed, the project is defining substrate activation pathways based on activation and stabilization of substrates at square planar molecules containing Al or Ga. The project trains a workforce of skilled synthetic inorganic chemists specializing in main group elements and in sustainable approaches to chemical synthesis. Collaborations with ACS Project SEED and the UC Davis NSF Research Experiences for Undergraduates (REU) site provide research mentoring and experience to economically-disadvantaged high school students and undergraduates, respectively.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.

在化学系化学合成项目的资助下，加州大学戴维斯分校的路易斯·伯本博士正在研究可持续元素铝的反应化学。这项工作为环保工业过程和先进制造提供了必要的见解。Berben博士正在积累的知识可以广泛应用于多相（即固态）和均相（即溶液）催化。该项目有助于建立环境和经济上可持续的化学工业，并有助于将原料有效地转化为增值化学品。其他影响还包括培养一支专门研究主要族元素的熟练合成无机化学家队伍，这是创造现代材料和电子产品所需要的，以及大规模化学合成的可持续方法。伯本博士还与国家项目合作，指导经济困难的高中生和本科生进行研究项目。这些拓展工作与她的科学贡献交织在一起。Berben博士正在探索铝（Al）和镓（Ga）的分子氧化还原活性配体配合物，以了解质子和电子转移产生氢化物等价物的机制，从而建立分子结构、热化学和氢化物转移反应活性之间的相关性。Berben博士也在探索这些反应的氧化还原介导的底物激活途径。具体的研究领域包括合成新的配体和金属配体分子，通过配体为基础的质子和电子转移化学介导氢化物等价物的产生。课题组通过pKa和水合值以及氢化物转移反应性来表征金属配体配合物，从而建立结构-性能-反应性的相关性。这些表征研究为反应条件的选择和新的分子设计提供了信息。基于正在开发的具有氧化还原活性的13族分子，该项目正在定义基于含有Al或Ga的方形平面分子的底物激活和稳定的底物激活途径。该项目培训了一支熟练的合成无机化学家队伍，专门研究主要族元素和可持续的化学合成方法。与ACS项目SEED和UC Davis NSF本科生研究经验（REU）网站的合作分别为经济困难的高中生和本科生提供研究指导和经验。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值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

期刊论文数量（7）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Syntheses of Square Planar Gallium Complexes and a Proton NMR Correlation Probing Metalloaromaticity

DOI：
10.1021/acs.inorgchem.0c01908
发表时间：
2020-09-21
期刊：
INORGANIC CHEMISTRY
影响因子：
4.6
作者：
Bass, Thomas M.;Carr, Cody R.;Berben, Louise A.
通讯作者：
Berben, Louise A.

Ligand Conjugation Directs the Formation of a 1,3-Dihydropyridinate Regioisomer

配体缀合引导 1,3-二氢吡啶酸酯区域异构体的形成

DOI：
10.1021/acs.inorgchem.0c02847
发表时间：
2020
期刊：
Inorganic Chemistry
影响因子：
4.6
作者：
Sherbow, Tobias J.;Parsons, Leo W.;Phan, Nathan A.;Fettinger, James C.;Berben, Louise A.
通讯作者：
Berben, Louise A.

A Ligand Protonation Series in Aluminum(III) Complexes of Tridentate Bis(enol)amine Ligand