Journal
NATURE CATALYSIS
Volume 2, Issue 2, Pages 149-156Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41929-018-0192-4
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Funding
- Army Research Office
- SABIC (Saudi Basic Industries Corporation)
- US Department of Energy (DOE) Office of Basic Energy Sciences
- US Department of Energy, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- US Department of Energy, Office of Biological and Environmental Research [49326]
- American Chemical Society Petroleum Research Fund [ACS PRF 55581-DNI5]
- [W911NF-16-1-0400]
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Supported single atoms provide an opportunity to design new heterogeneous catalysts while optimizing the utilization of noble metals. However, identification of the active single-atom structure is required for understanding the reaction mechanism and guiding catalyst design. Here, we use in situ infrared spectroscopy, operando X-ray absorption spectroscopy and quantum chemical calculations to identify the active single-atom complex as well as the resting state of the Ir/MgAl2O4 catalysts during the low-temperature CO oxidation. In contrast to poisoning of iridium nanoparticles by CO, here we show that the formation of Ir(CO) on single atoms results in a different reaction mechanism and high activity for low-temperature CO oxidation. This is due to the ability of single atoms to coordinate with multiple ligands, where Ir(CO) provides an interfacial site for facile O-2 activation between Ir and Al and lowers the reaction barrier between gas-phase CO(g) and *O in Ir(CO)(O) through an Eley-Rideal mechanism.
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