Spectroscopic determination of metal redox and segregation effects during CO and CO/NO oxidation over silica-supported Pd and PdCu catalysts

Kristy, Stephen; Svadlenak, Scott; Hoffman, Adam S.; Bare, Simon R.; Goulas, Konstantinos A.

doi:10.1016/j.apcatb.2023.123329

Title: Spectroscopic determination of metal redox and segregation effects during CO and CO/NO oxidation over silica-supported Pd and PdCu catalysts

Journal Article · 26 September 2023 · Applied Catalysis. B, Environmental

DOI: https://doi.org/10.1016/j.apcatb.2023.123329 · OSTI ID:2327108

^[1]; Svadlenak, Scott ^[2]; Hoffman, Adam S. ^[3]; Bare, Simon R. ^[3]; Goulas, Konstantinos A. ^[2]

Oregon State Univ., Corvallis, OR (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Oregon State Univ., Corvallis, OR (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Here, we report the effects of alloying Cu into silica supported Pd nanoparticles on the catalytic activity, surface composition, and particle structure during CO oxidation Pd is highly active for CO oxidation but is inhibited by relevant competitive reagents (e.g. NO) at low temperatures (< 150 °C). By alloying Cu into Pd nanoparticles, NO inhibition is suppressed without any CO oxidation activity loss. Infrared spectroscopy illustrates the formation of surface nitrosyl (NO-Pd) is eliminated in the PdCu alloy catalyst, preventing CO oxidation inhibition by NO. X-ray absorption spectroscopy studies show that Pd in the monometallic catalyst forms a surface oxide after light-off. Conversely, in the PdCu catalyst, Pd remains metallic during reaction, independent of temperature, whereas the Cu oxidizes when the catalyst becomes active, after light-off. Furthermore, DRIFTS studies show that the Cu segregates to the surface as the catalyst becomes active for diesel oxidation, presumably becoming the O₂ adsorption site.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Oak Ridge Institute for Science and Education (ORISE), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-76SF00515; SC0014664

OSTI ID:: 2327108

Journal Information:: Applied Catalysis. B, Environmental, Vol. 342; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
diesel oxidation catalysis
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operando X-ray absorption spectroscopy
operando infrared spectroscopy

Title: Spectroscopic determination of metal redox and segregation effects during CO and CO/NO oxidation over silica-supported Pd and PdCu catalysts

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