Enabling Redox Reactions for Catalysis with Group 13 Elements

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丝·伯本博士正在研究可持续元素铝的反应化学。这项工作为环境友好型工业流程和先进制造提供了必要的洞察力。伯本博士正在产生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，并有效地将原料转化为增值化学品。其他影响是培养一支熟练的合成无机化学家队伍，专门研究主族元素，这是创造现代材料和电子产品所需的，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，在研究项目中指导经济困难的高中生和本科生。这些外展努力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络合物，以了解质子和电子转移生成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的反应性之间的关联。伯本博士还在为这些反应探索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，它们通过基于配体的质子和电子转移化学来调节氢化物等价物的生成。该课题组通过pKa和水合度以及氢化物转移反应性表征了金属-配体络合物，从而建立了结构-性质-反应性的关联。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。在正在开发的氧化还原活性基团13分子的基础上，该项目正在定义基于含有Al或Ga的正方形平面分子上底物的激活和稳定的底物激活途径。该项目培养了一支熟练的合成无机化学家队伍，专门从事主族元素和可持续化学合成方法的研究。与美国大学戴维斯分校的SEED项目和加州大学戴维斯分校本科生研究体验(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。

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.