Atomically Dispersed Pd–O Species on CeO2(111) as Highly Active Sites for Low-Temperature CO Oxidation

Spezzati, Giulia; Su, Yaqiong; Hofmann, Jan P.; Benavidez, Angelica D.; DeLaRiva, Andrew T.; McCabe, Jay; Datye, Abhaya K.; Hensen, Emiel J. M.

doi:10.1021/acscatal.7b02001

Title: Atomically Dispersed Pd–O Species on CeO₂(111) as Highly Active Sites for Low-Temperature CO Oxidation

Journal Article · Thu Sep 07 00:00:00 UTC 2017 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.7b02001 · OSTI ID:1414915

Spezzati, Giulia ^[1]; Su, Yaqiong ^[2];

^[2]; Benavidez, Angelica D. ^[3]; DeLaRiva, Andrew T. ^[3]; McCabe, Jay ^[3]; Datye, Abhaya K. ^[3];

^[2]

Eindhoven Univ. of Technology, Eindhoven (The Netherlands); The Netherlands Organization for Scientific Research (NWO)
Eindhoven Univ. of Technology, Eindhoven (The Netherlands)
Univ. of New Mexico, Albuquerque, NM (United States)

Ceria-supported Pd is a promising heterogeneous catalyst for CO oxidation relevant to environmental cleanup reactions. Pd loaded onto a nanorod form of ceria exposing predominantly (111) facets is already active at 50 °C. Here we report a combination of CO-FTIR spectroscopy and theoretical calculations that allows assigning different forms of Pd on the CeO₂(111) surface during reaction conditions. Single Pd atoms stabilized in the form of PdO and PdO₂ in a CO/O₂ atmosphere participate in a catalytic cycle involving very low activation barriers for CO oxidation. In conclusion, the presence of single Pd atoms on the Pd/CeO₂-nanorod, corroborated by aberration-corrected TEM and CO-FTIR spectroscopy, is considered pivotal to its high CO oxidation activity.

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Research Organization:: The Netherlands Organization for Scientific Research (NWO) (The Netherlands); Univ. of New Mexico, Albuquerque, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FG02-05ER15712

OSTI ID:: 1414915

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 10 Vol. 7; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO oxidation
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computational modeling
mechanism
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Title: Atomically Dispersed Pd–O Species on CeO2(111) as Highly Active Sites for Low-Temperature CO Oxidation

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Title: Atomically Dispersed Pd–O Species on CeO₂(111) as Highly Active Sites for Low-Temperature CO Oxidation