Dissertation Defense: Arvin Kakekhani, Yale University, “Using Ferroelectrics to Tackle Fundamental Challenges in Catalysis”

Surface catalysis based on transition metals and their alloys has been one of the most important research fields in theoretical and experimental catalysis and chemistry. Recently, the development of a microscopic theoretical framework combined with the computational capability and accuracy of first principles calculations has changed the nature of this field from a largely trial and error approach to a predictive and controlled design process. In addition to deepening our knowledge of catalysis at the microscopic scale and helping design improved catalysts for important chemical reactions, this framework for heterogeneous catalysis has helped us understand some of the fundamental limitations of the catalytic activities of current materials and processes. In this thesis, we briefly introduce these limitations and their root causes in terms of electronic and structural properties. Next, we describe how using ferroelectric surfaces and exploiting their polarization dependent switchable surface chemistry can tackle some of these fundamental challenges. We then design processes and materials that can catalyze reactions that are considered challenging (if not near impossible) using current catalytic materials and processes. As specific examples, we discuss the possibility of using ferroelectric-based materials to catalyze industrially and environmentally important reactions including water splitting, direct NO$_{x}$ decomposition, and partial oxidation of methane to methanol.