Enabling Redox Reactions for Catalysis with Group 13 Elements

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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.