Developing a mechanistic understanding of CO oxidation catalysts is a challenging issue that continues to be of interest to industry and academia. Effective oxidation of CO is important towards the development of catalytic converters for automotive and stationary power sources and carbon-neutral synthetic fuel production. Recent work by the PIs demonstrates that the incorporation of multi-dimensional defects, such as dislocations (1D) and stacking faults (2D), into ceramic materials can dramatically change their reducibility and ability to donate oxygen for catalytic purposes. Although limited work exists studying the effect of point defects (0D) on catalytic activity, its extension to multi-dimensional defects (1D, 2D) remains to be undertaken. Here, experimental (Rosen) and computational (Rondinelli) studies will assess the feasibility of engineering 1D and 2D defects into catalyst supports to modulate oxygen donation and CO oxidation kinetics. We will study cerium oxide and cerium/lanthanum-based perovskites (Ce,La)BO3. In-situ XRD under reactive environments and high-temperature TEM will be used to study the redox behavior and the dynamics of engineered defects. The electronic structures and energies of pristine/defective materials both with and without H2/CO will be calculated using state-of-the-art density functional theory (DFT) and thermodynamic and kinetic models. In previous DFT studies on perovskite defects, it was difficult to accurately consider the complexities in experimental samples, while, in this project, Rosen's experimental characterization can provide Rondinelli the essential information about the sample bulks and surfaces. The integrated feedback between experiment and theory will provide new understanding for the future deterministic design of improved CO oxidation materials.
|Effective start/end date||10/1/17 → 9/30/19|
- United States-Israel Binational Science Foundation (2016079)