Effects of Molecular and Electronic Structures in CoOx/CeO2 Catalysts on NO Reduction by CO

Zhang, Shuhao; Li, Yuanyuan; Huang, Jiahao; Lee, Jaeha; Kim, Do Heui; Frenkel, Anatoly I.; Kim, Taejin

doi:10.1021/acs.jpcc.8b12442

Title: Effects of Molecular and Electronic Structures in CoO_x/CeO₂ Catalysts on NO Reduction by CO

Journal Article · Mon Mar 04 00:00:00 EST 2019 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.8b12442· OSTI ID:1508522

^[1]; Li, Yuanyuan ^[1]; Huang, Jiahao ^[1]; Lee, Jaeha ^[2]; Kim, Do Heui ^[2];

^[3];

^[1]

Stony Brook Univ., Stony Brook, NY (United States)
Seoul National Univ., Seoul (Republic of Korea)
Stony Brook Univ., Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Ceria-supported transition metal oxide (such as CoO_x) catalysts are promising, more cost-effective candidates to replace platinum group metal catalysts in the NO reduction process. A series of CoO_x (0.2–31.3 Co/nm²) catalysts supported on CeO₂ were prepared by the incipient wetness impregnation method and were tested for NO reduction by CO reaction in this work. Various characterization techniques, including Brunauer–Emmett–Teller, Raman spectroscopy, powder X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) were used to investigate the molecular and electronic structures of CoO_x/CeO₂ catalysts. It was observed that there are structural changes with varied Co loadings, such as (1) sub-monolayer: <2.3 Co/nm², (2) monolayer: 2.3–2.7 Co/nm², and (3) over-monolayer: >2.7 Co/nm². The highest molar rate was observed at the 2.7 Co/nm2 sample. In the case of over-monolayer samples, such as 7.1 Co/nm², the oxidation state of Co affected the catalytic activity. Using in situ XAS, an oxidation state change from Co³⁺ to Co²⁺ between 200 and 300 °C was identified. Catalyst deactivation was also affected by the change of Co oxidation states from the fresh sample (Co³⁺) to the used sample (Co³⁺/Co²⁺). N₂O formation and decomposition were affected by the reaction temperature in a two-step procedure, where NO converts into N₂: (1) NO → N₂O and (2) N₂O → N₂. N₂ selectivity monotonically increased with an increasing reaction temperature between 200 and 400 °C. Furthermore, the results provided several structure–property relationships and a possible reaction mechanism for NO reduction by CO reaction over CoO_x/CeO₂ catalysts.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1508522

Report Number(s):: BNL-211570-2019-JAAM

Journal Information:: Journal of Physical Chemistry. C, Vol. 123, Issue 12; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 23 works

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