Guest Seminar - Computational Catalysis for Problems in Energy and Sustainability

The rapid development of modern society has been met by a fierce and overwhelming increase in fossil fuel utilization and the mass production of nonrenewable/ recyclable materials. For a sustainable future, it is imperative that we develop methods that harness “green” electrons to convert harmful greenhouse gases towards useful fuels. Working hand-in-hand with experimental collaborators, we leverage electronic structure calculations to propose and validate several remarkable catalytic platforms. We first explore the conversion of CO2 to methanol catalyzed by Cobalt Phthalocyanine (CoPc) immobilized on carbon nanotubes (CNTs). We prove experimentally and elucidate computationally how increased curvature of single-walled CNTs can steer the selectivity from undesired CO towards desired methanol. When then apply this concept to Iron Phthalocyanine (FePc) for oxygen reduction, demonstrating how molecular curvature induced by the single-walled CNT support translates to accelerated electron transfer and enhanced catalytic performance. Using CoPc and FePc as inspiration, we screen a series of phthalocyanine-based dual atom catalysts (DACs) for the efficient conversion of CO to ethylene. We find the DACs’ intrinsically strained nature enables facile dimerization of CO molecules, which is traditionally the rate-limiting step for multi-carbon product formation. Finally, we explore surface-doped Ruthenium oxide (X-RuO2) catalysts for acidic oxygen evolution. Our calculations reveal several stability-enhancing dopants when embedded in the RuO2 matrix. The improved durability is attributed to the dopant’s ability to shut down reaction pathways that generate defects in the catalyst.