Identification of the active complex for CO oxidation over single-atom Ir-on-MgAl2O4 catalysts

Lu, Yubing; Wang, Jiamin; Yu, Liang; Kovarik, Libor; Zhang, Xiwen; Hoffman, Adam S.; Gallo, Alessandro; Bare, Simon R.; Sokaras, Dimosthenis; Kroll, Thomas; Dagle, Vanessa; Xin, Hongliang; Karim, Ayman M.

doi:10.1038/s41929-018-0192-4

Title: Identification of the active complex for CO oxidation over single-atom Ir-on-MgAl₂O₄ catalysts

Journal Article · Mon Dec 31 00:00:00 EST 2018 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-018-0192-4· OSTI ID:1503098

^[1]; Wang, Jiamin ^[1]; Yu, Liang ^[1]; Kovarik, Libor ^[2]; Zhang, Xiwen ^[1]; Hoffman, Adam S. ^[3]; Gallo, Alessandro ^[4]; Bare, Simon R. ^[3]; Sokaras, Dimosthenis ^[3]; Kroll, Thomas ^[3]; Dagle, Vanessa ^[2]; Xin, Hongliang ^[1];

^[1]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Supported single atoms provide the best utilization of noble metals and provide an opportunity to design new heterogeneous catalysts. However, identification of the active single atoms structure is required for understanding the reaction mechanism and guiding catalyst design. We used in-situ infrared spectroscopy, in-operando x-ray adsorption spectroscopy and quantum chemical calculations to show that Ir(CO)/MgAl2O4 is the active single atom complex for low temperature CO oxidation and Ir(CO)(O) is the most stable intermediate. In contrast to poisoning of nanoparticles by CO, 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 CO, in Ir(CO)(O), acts as a facilitator by lowering the reaction barrier between gas phase CO and adsorbed O (Eley-Rideal mechanism).

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515; AC05-76RL01830

OSTI ID:: 1503098

Alternate ID(s):: OSTI ID: 1502401

Report Number(s):: PNNL-SA-138518

Journal Information:: Nature Catalysis, Vol. 2, Issue 2; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 171 works

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