Transition metal atoms isolated in the surface of nitrogen-doped carbon have demonstrated excellent thermocatalytic and electrocatalytic performance, most notably in reactions involving oxygen. In the current work, the low temperature thermocatalytic oxidation of carbon monoxide was studied over Co atoms isolated in a nitrogen-doped carbon support. Steady-state isotopic transient kinetic analysis revealed a high turnover frequency of the reaction at 273 K with a simultaneous low surface coverage of reactive intermediates leading to CO2. A new proposed reaction path for low temperature CO oxidation on these materials is consistent with the observed kinetics of the reaction (orders of reaction and apparent activation energy), the calculated energetics of elementary steps evaluated by density functional theory (DFT) and the reaction progress followed by ab initio molecular dynamics. The magnitude of DFT-calculated reactant adsorption energies on other isolated metal atoms in nitrogen-doped carbon suggested Rh would also be a good catalyst for low-temperature CO oxidation. Experimentally measured reaction kinetics over the isolated Rh atoms are consistent with the new reaction path.
Robert Davis obtained his Ph.D. degree in Chemical Engineering from Stanford University in 1989. He subsequently worked as a postdoctoral research fellow in the Chemistry Department at the University of Namur in Belgium. He joined the faculty in Chemical Engineering at the University of Virginia in 1990 and is currently the William Stansfield Calcott Professor. Professor Davis also served as the Chair of Chemical Engineering at the University of Virginia from 2002 to 2011. He received the Wilhelm Award of the AICHE, the Emmett Award of the North American Catalysis Society, the NSF Young Investigator Award, the DuPont Young Professor Award, the Union Carbide Innovation Recognition Award, and the UVA Rodman Scholars Award for Excellence in Teaching. Professor Davis has served as President of the Southeastern Catalysis Society, Chair of the 2006 Gordon Research Conference on Catalysis, Chair of Catalysis Programming of the AIChE, Chair of a US government panel charged with worldwide assessment of Catalysis by Nanostructured Materials, Director of the Catalysis and Reaction Engineering Division of the AIChE, Director of the North American Catalysis Society, Co-Chair of an International Catalysis Workshop in China, member of the Advisory Board of the International Conferences on Solid Acid and Base Catalysis, and member of the editorial boards of Journal of Catalysis, Applied Catalysis A and B, Molecular Catalysis, ChemCatChem and ACS Catalysis.
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