Relating adatom emission to improved durability of Pt-Pd diesel oxidation catalysts
Abstract
Sintering of nanoparticles is an important contributor to loss of activity in heterogeneous catalysts, such as those used for controlling harmful emissions from automobiles. But mechanistic details, such as the rates of atom emission or the nature of the mobile species, remain poorly understood. Herein we report a novel approach that allows direct measurement of atom emission from nanoparticles. We use model catalyst samples and a novel reactor that allows the same region of the sample to be observed after short-term heat treatments (seconds) under conditions relevant to diesel oxidation catalysts (DOCs). Monometallic Pd is very stable and does not sinter when heated in air (T ≤ 800 °C). Pt sinters readily in air, and at high temperatures (≥800 °C) mobile Pt species emitted to the vapor phase cause the formation of large, faceted particles. In Pt–Pd nanoparticles, Pd slows the rate of emission of atoms to the vapor phase due to the formation of an alloy. However, the role of Pd in Pt DOCs in air is quite complex: at low temperatures, Pt enhances the rate of Pd sintering (which otherwise would be stable as an oxide), while at higher temperature Pd helps to slow the rate of Ptmore »
- Authors:
-
- Univ. of New Mexico, Albuquerque, NM (United States)
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Einhoven Univ. of Technology, Eindhoven (The Netherlands)
- New Mexico State Univ., Las Cruces, NM (United States)
- General Motors Global R&D, Warren, MI (United States)
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1235327
- Alternate Identifier(s):
- OSTI ID: 1434176
- Report Number(s):
- SAND-2015-4863J
Journal ID: ISSN 0021-9517; 594892
- Grant/Contract Number:
- AC04-94AL85000
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Catalysis
- Additional Journal Information:
- Journal Volume: 328; Journal Issue: C; Journal ID: ISSN 0021-9517
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; adatom emission; Ostwald ripening; catalyst sintering; Pt–Pd; diesel oxidation; exhaust treatment
Citation Formats
Johns, Tyne Richele, Goeke, Ronald S., Ashbacher, Valerie, Thune, Peter C., Niemantsverdriet, J. W., Kiefer, Boris, Kim, Chang H., Balogh, Michael P., and Datye, Abhaya K. Relating adatom emission to improved durability of Pt-Pd diesel oxidation catalysts. United States: N. p., 2015.
Web. doi:10.1016/j.jcat.2015.03.016.
Johns, Tyne Richele, Goeke, Ronald S., Ashbacher, Valerie, Thune, Peter C., Niemantsverdriet, J. W., Kiefer, Boris, Kim, Chang H., Balogh, Michael P., & Datye, Abhaya K. Relating adatom emission to improved durability of Pt-Pd diesel oxidation catalysts. United States. https://doi.org/10.1016/j.jcat.2015.03.016
Johns, Tyne Richele, Goeke, Ronald S., Ashbacher, Valerie, Thune, Peter C., Niemantsverdriet, J. W., Kiefer, Boris, Kim, Chang H., Balogh, Michael P., and Datye, Abhaya K. Fri .
"Relating adatom emission to improved durability of Pt-Pd diesel oxidation catalysts". United States. https://doi.org/10.1016/j.jcat.2015.03.016. https://www.osti.gov/servlets/purl/1235327.
@article{osti_1235327,
title = {Relating adatom emission to improved durability of Pt-Pd diesel oxidation catalysts},
author = {Johns, Tyne Richele and Goeke, Ronald S. and Ashbacher, Valerie and Thune, Peter C. and Niemantsverdriet, J. W. and Kiefer, Boris and Kim, Chang H. and Balogh, Michael P. and Datye, Abhaya K.},
abstractNote = {Sintering of nanoparticles is an important contributor to loss of activity in heterogeneous catalysts, such as those used for controlling harmful emissions from automobiles. But mechanistic details, such as the rates of atom emission or the nature of the mobile species, remain poorly understood. Herein we report a novel approach that allows direct measurement of atom emission from nanoparticles. We use model catalyst samples and a novel reactor that allows the same region of the sample to be observed after short-term heat treatments (seconds) under conditions relevant to diesel oxidation catalysts (DOCs). Monometallic Pd is very stable and does not sinter when heated in air (T ≤ 800 °C). Pt sinters readily in air, and at high temperatures (≥800 °C) mobile Pt species emitted to the vapor phase cause the formation of large, faceted particles. In Pt–Pd nanoparticles, Pd slows the rate of emission of atoms to the vapor phase due to the formation of an alloy. However, the role of Pd in Pt DOCs in air is quite complex: at low temperatures, Pt enhances the rate of Pd sintering (which otherwise would be stable as an oxide), while at higher temperature Pd helps to slow the rate of Pt sintering. DFT calculations show that the barrier for atom emission to the vapor phase is much greater than the barrier for emitting atoms to the support. Thus, vapor-phase transport becomes significant only at high temperatures while diffusion of adatoms on the support dominates at lower temperatures.},
doi = {10.1016/j.jcat.2015.03.016},
journal = {Journal of Catalysis},
number = C,
volume = 328,
place = {United States},
year = {Fri Jun 05 00:00:00 EDT 2015},
month = {Fri Jun 05 00:00:00 EDT 2015}
}
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