Journal Article PUBDB-2025-04555

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Complementary and Spatially Resolved Operando Spectroscopic Investigation of Pt/Al$_2$O$_3$ and Pt/CeO$_2$ Catalysts during CO/NO Conversion

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2025
Soc. Washington, DC

The journal of physical chemistry / C 129(31), 13923 - 13938 () [10.1021/acs.jpcc.5c01963]
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Abstract: The composition of reaction mixtures strongly influences the structural evolution and performance of noble metal-based catalysts. In this work, we compared the effect of the simultaneous presence of CO and NO on the noble metal state and CO oxidation activity of Pt/Al$_2$O$_3$ and Pt/CeO$_2$ catalysts under close-to-stoichiometric conditions using complementary in situ/operando X-ray and infrared spectroscopic techniques. For the utilized catalysts, the integral catalytic performance data indicated a diminished CO oxidation activity in the presence of NO, which is due to a competitive adsorption of CO and NO, as elucidated by the diffuse reflectance infrared Fourier transform spectroscopy and high-energy resolution X-ray fluorescence X-ray absorption near-edge structure results. Spatially resolved operando X-ray absorption spectroscopy investigations and extended X-ray absorption fine structure analysis unraveled that the addition of NO led to a higher oxidation state of Pt along the entire catalyst bed for both samples. Moreover, NO was found to delay the reduction of Pt particles on Al$_2$O$_3$ and hinder the formation of active Pt clusters on CeO$_2$. As a result, a more oxidized Pt state at the beginning of the catalyst bed and a low overall activity were observed for Pt/CeO$_2$. However, the CO oxidation activity could be enhanced by a reductive pretreatment of the Pt/CeO$_2$ catalyst, resulting in a similar reduced Pt state along the entire catalyst bed and minimizing the negative impact of NO during the combined reaction.

Classification:

Contributing Institute(s):
  1. DOOR-User (DOOR ; HAS-User)
Research Program(s):
  1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
  2. SFB 1441 A03 - Reaktivität und hochentwickelte Elektronenmikroskopie von massenselektierten Clustern auf Oxidträgern (A03) (446697387) (446697387)
  3. SFB 1441 B01 - Synthese und Charakterisierung von Metalloxidträgern mit hoher Oberfläche (B01) (446700158) (446700158)
  4. SFB 1441 B02 - Systematische Synthese und katalytische Tests von definierten Edelmetallspezies auf Pulverträgern (B02) (446700275) (446700275)
  5. SFB 1441 B03 - In situ/operando-Charakterisierung von Edelmetallclustern und Partikeln auf Metalloxiden unter Reaktionsbedingungen (B03) (446701131) (446701131)
  6. SFB 1441 C04 - Orts- und Zeitaufgelöste Untersuchung der Gasphase und der Struktur des Katalysators (C04) (446711557) (446711557)
  7. FS-Proposal: I-20210886 (I-20210886) (I-20210886)
  8. DFG project G:(GEPRIS)460248799 - DAPHNE4NFDI - DAten aus PHoton- und Neutronen Experimenten für NFDI (460248799) (460248799)
Experiment(s):
  1. PETRA Beamline P65 (PETRA III)

Appears in the scientific report 2025
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 Record created 2025-10-23, last modified 2025-12-02


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