CAS: Computational Modeling of Carbon Monoxide Dehydrogenase Model Systems for Carbon Dioxide Fixation

Suny At Binghamton, Binghamton NY

Investigators

Abstract

With support from the Chemical Structure, Dynamics & Mechanisms B Program of the Chemistry Division, Professor Julien Panetier and his students in the Department of Chemistry at Binghamton University are designing molecular catalysts that use renewable electricity to reduce carbon dioxide (CO2) to higher energy-reduced carbon compounds. This research aims to computationally study earth-abundant materials that mimic essential structural features and functions of metalloenzymes, such as carbon monoxide dehydrogenases, to contribute to the rational design of bioinspired CO2 reduction electrocatalysts. This project will also engage Binghamton High School students in hands-on laboratory experiments on renewable and sustainable energy. The goal is to foster a learning environment in which students, particularly underrepresented minorities, have a higher likelihood of graduating and being retained in STEM (science, technology, engineering, and mathematics) education. Under this award, the research team led by Professor Julien Panetier at Binghamton University aims to study computationally molecular electrocatalysts that mimic essential structural features and functions of Ni,Fe-carbon monoxide dehydrogenases (Ni,Fe-CODHs) to rationally design bioinspired molecular electrocatalysts for CO2 reduction over H+ reduction using H2O as the proton source. In this project, the team will focus on 1) understanding the synergy between redox-active macrocycle ligands and transition metal ions in CODH model systems to enhance selectivity for CO2-to-CO conversion, 2) investigating the mechanistic impact and design principles of second-sphere ligands to alter the linear free-energy relationship between overpotential and turnover frequency, and 3) validating our computational predictions by benchmarking our results with empirical data and collaborating with experimentalists. The mechanistic understanding and design of CODH model systems will fundamentally advance the sustainable and renewable energy field and have a broad scientific impact on enzymatic catalysis. 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.