Interparticle Metal-Metal Interactions in Electrocatalytic Carbon Dioxide Reduction Reactions

Yale University, New Haven CT

Investigators

Abstract

A major challenge in the transition to clean energy is reducing emissions of carbon dioxide from fuel combustion. Using renewable electricity to convert carbon dioxide to value-added fuels and chemical products is a promising way of turning carbon emissions into a resource. Palladium is a unique metal that can catalyze the electrochemical conversion of carbon dioxide to formate ion (HCOO-). Formate is a building-block compound that can be used to produce industrially important chemicals such as formaldehyde and methanol. The catalytic performance of palladium, however, is severely limited by rapid deactivation of the catalyst active site, and it is difficult to design improved systems without further understanding of both the reaction and deactivation mechanisms. This research project will study novel catalysts composed of palladium and a secondary metal. The aim is to stabilize the catalyst active site and thereby develop catalysts can perform the sustained, efficient conversion of carbon dioxide into formate. This research project also will foster new teaching and learning opportunities for a large and diverse body of students. The aim of this research project is to investigate how nanoscale interparticle metal-metal interactions influence the catalytic mechanisms of carbon dioxide electroreduction on palladium. The goals are to limit catalyst deactivation during the production of formate and to enable the synthesis of new products such as formaldehyde or methanol. Metal nanoparticles will be used as “electronic ligands” and modify the binding strength of palladium with reaction intermediates. The nanoparticles also can act as “collaborative ligands” that directly participate in catalysis by providing a secondary type of surface site. The electronic and collaborative interactions between palladium and a variety of other metals will be studied. Additionally, experiments will be performed to learn how these interactions change the binding energetics of palladium with the reaction intermediates and the potential-dependent reduction reaction pathways. Ultimately, the knowledge gained from these studies will be used to develop electrocatalysts that are stable for efficient conversion of carbon dioxide to formate and then on to more complex products. 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.