Multi-electron Multi-proton Catalysis using Electron-coupled-proton Buffers Based on 3d Transition Metals and Redox-active Ligands

With the support of the Chemical Catalysis Program in the Division of Chemistry, Professor Isaac Garcia-Bosch at Carnegie Mellon University is studying metal complexes bearing redox-active ligands (electron-coupled proton buffers, ECPBs) that perform multi-electron multi-proton transformations. The goal of this research is to use these new complexes to perform challenging reactions in a selective fashion and under mild conditions. This project will lead to a better understanding of ubiquitous reactions in biological and industrial processes, and contribute to the design of new catalysts based on cheap metals such as copper or iron. During the execution of this project, several graduate and undergraduate students at Carnegie Mellon University will be trained in the synthesis and characterization of metal complexes, as well as study reaction mechanisms. The project also includes scientific collaborations with renowned experts in the field of spectroscopy and computational chemistry. Outreach activities in elementary schools and high-schools in the Pittsburgh area will be carried out, benefitting K-12 students with limited access to science. With the support of the Chemical Catalysis Program in the Division of Chemistry, Professor Isaac Garcia-Bosch at Carnegie Mellon University is studying fundamental questions regarding the geometry, electronic structure, spectroscopy, and reactivity of ECPBs based on 3d metals and redox-active ligands. Current project activities include 1) synthesis and characterization of ECPBs in different protonation/oxidation states; 2) study of the thermochemistry of ECPB reactivity; and 3) the use of ECPBs to promote substrate oxidation (using O2 and H2O2 as oxidants) and substrate reduction (using H2 and N2H4 as reductants). The results of these activities will provide fundamental knowledge on metal-ligand cooperativity, leading to the development of efficient, practical, and selective catalysts based on 1st row transition metals. The work will be presented at research conferences and reported in scientific journals. 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.