Palladium oxidation leads to methane combustion activity: Effects of particle size and alloying with platinum
Abstract
Pd- and Pt-based catalysts are highly studied materials due to their widespread use in emissions control catalysis. However, claims continue to vary regarding the active phase and oxidation state of the metals. Different conclusions have likely been reached due to the heterogeneous nature of such materials containing various metal nanoparticle sizes and compositions, which may each possess unique redox features. In this work, using uniform nanocrystal catalysts, we study the effect of particle size and alloying on redox properties of Pd-based catalysts and show their contribution to methane combustion activity using operando quick extended x-ray absorption fine structure measurements. Results demonstrate that for all studied Pd sizes (3 nm–16 nm), Pd oxidation directly precedes CH4 combustion to CO2, suggesting Pd oxidation as a prerequisite step to methane combustion, and an oxidation pretreatment shows equal or better catalysis than a reduction pretreatment. Results are then extended herein to uniform alloyed PtxPd1–x nanoparticles, where oxidative pretreatments are shown to enhance low-temperature combustion. In these uniform alloys, we observe a composition-dependent effect with Pt-rich alloys showing the maximum difference between oxidative and reductive pretreatments. In Pt-rich alloys, we initially observe that the presence of Pt maintains Pd in a lower-activity reduced state. However,more »
- Authors:
-
- Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis and Dept. of Chemical Engineering
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry and National Center for Electron Microscopy
- Paul Scherrer Institute, Villigen, Switzerland
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1596989
- Alternate Identifier(s):
- OSTI ID: 1570868
- Grant/Contract Number:
- ECCS-1542152; DGE-1656518; AC02-76SF00515; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 151; Journal Issue: 15; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Goodman, Emmett D., Ye, Angela A., Aitbekova, Aisulu, Mueller, Oliver, Riscoe, Andrew R., Nguyen Taylor, Temy, Hoffman, Adam S., Boubnov, Alexey, Bustillo, Karen C., Nachtegaal, Maarten, Bare, Simon R., and Cargnello, Matteo. Palladium oxidation leads to methane combustion activity: Effects of particle size and alloying with platinum. United States: N. p., 2019.
Web. doi:10.1063/1.5126219.
Goodman, Emmett D., Ye, Angela A., Aitbekova, Aisulu, Mueller, Oliver, Riscoe, Andrew R., Nguyen Taylor, Temy, Hoffman, Adam S., Boubnov, Alexey, Bustillo, Karen C., Nachtegaal, Maarten, Bare, Simon R., & Cargnello, Matteo. Palladium oxidation leads to methane combustion activity: Effects of particle size and alloying with platinum. United States. https://doi.org/10.1063/1.5126219
Goodman, Emmett D., Ye, Angela A., Aitbekova, Aisulu, Mueller, Oliver, Riscoe, Andrew R., Nguyen Taylor, Temy, Hoffman, Adam S., Boubnov, Alexey, Bustillo, Karen C., Nachtegaal, Maarten, Bare, Simon R., and Cargnello, Matteo. Fri .
"Palladium oxidation leads to methane combustion activity: Effects of particle size and alloying with platinum". United States. https://doi.org/10.1063/1.5126219. https://www.osti.gov/servlets/purl/1596989.
@article{osti_1596989,
title = {Palladium oxidation leads to methane combustion activity: Effects of particle size and alloying with platinum},
author = {Goodman, Emmett D. and Ye, Angela A. and Aitbekova, Aisulu and Mueller, Oliver and Riscoe, Andrew R. and Nguyen Taylor, Temy and Hoffman, Adam S. and Boubnov, Alexey and Bustillo, Karen C. and Nachtegaal, Maarten and Bare, Simon R. and Cargnello, Matteo},
abstractNote = {Pd- and Pt-based catalysts are highly studied materials due to their widespread use in emissions control catalysis. However, claims continue to vary regarding the active phase and oxidation state of the metals. Different conclusions have likely been reached due to the heterogeneous nature of such materials containing various metal nanoparticle sizes and compositions, which may each possess unique redox features. In this work, using uniform nanocrystal catalysts, we study the effect of particle size and alloying on redox properties of Pd-based catalysts and show their contribution to methane combustion activity using operando quick extended x-ray absorption fine structure measurements. Results demonstrate that for all studied Pd sizes (3 nm–16 nm), Pd oxidation directly precedes CH4 combustion to CO2, suggesting Pd oxidation as a prerequisite step to methane combustion, and an oxidation pretreatment shows equal or better catalysis than a reduction pretreatment. Results are then extended herein to uniform alloyed PtxPd1–x nanoparticles, where oxidative pretreatments are shown to enhance low-temperature combustion. In these uniform alloys, we observe a composition-dependent effect with Pt-rich alloys showing the maximum difference between oxidative and reductive pretreatments. In Pt-rich alloys, we initially observe that the presence of Pt maintains Pd in a lower-activity reduced state. However, with time on stream, PdO eventually segregates under oxidizing combustion conditions, leading to a slowly increasing activity. Overall, across particle sizes and alloy compositions, we relate increased catalytic activity to Pd oxidation, thus shedding light on previous contrasting results related to the methane combustion activity of these catalysts.},
doi = {10.1063/1.5126219},
journal = {Journal of Chemical Physics},
number = 15,
volume = 151,
place = {United States},
year = {2019},
month = {10}
}
Web of Science
Figures / Tables:

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