1950
Plasmon Enhancement of the CO Oxidation Reaction over Supported Gold Catalysts

Wednesday, 3 October 2018
Universal Ballroom (Expo Center)
P. Novello, J. Liu (Duke University), and P. Varanasi (Materials Science Division, U.S. Army Research Office, Duke University)
An active catalyst for the oxidation of CO at all temperatures is essential to ensuring safer air quality. In this study, we demonstrate the use of light to enhance CO oxidation over supported plasmonic gold catalysts, resulting in high activity and more substantial lifetimes at all temperatures ranging from -50 to 250 ֯C. Catalysts are synthesized by impregnation with plasmonic gold nanoparticles with a known size and plasmon resonance frequency. Using experiments which couple light induced desorption of CO2 and regeneration of catalytic activity, we propose a mechanism for light enhancement of gold catalysis. The reaction mechanism is strongly affected by the interaction between hot-electrons generated from relaxation of localized surface plasmon resonances in Au nanoparticles and adjacent species as well as photothermal heating. Through a separation of photothermal heating effects from hot-electron effects, we demonstrate an effective catalyst heating of over 70 oC and an additional nonthermal improvement of catalytic activity surpassing 100%. The hot-electron effects are shown to reactivate gold catalysts by removing surface carbonates which otherwise form in the active sites and poison the catalyst. This more efficient application allows for dramatically increased catalytic activity and catalyst lifetime, demonstrating a new path for highly active CO oxidation and further insight into light and hot-electron enhanced catalysis.