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Palladium oxidation leads to methane combustion activity: Effects of particle size and alloying with platinum

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.5126219· OSTI ID:1596989
 [1];  [1];  [1];  [2];  [1];  [1];  [2];  [2];  [3];  [4];  [2];  [1]
  1. Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis and Dept. of Chemical Engineering
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry and National Center for Electron Microscopy
  4. Paul Scherrer Institute, Villigen, Switzerland
+ Show Author Affiliations

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.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231
OSTI ID:
1596989
Alternate ID(s):
OSTI ID: 1570868
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 15 Vol. 151; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (2)

Understanding the Role of SnO 2 Support in Water‐Tolerant Methane Combustion: In situ Observation of Pd(OH) 2 and Comparison with Pd/Al 2 O 3 journal December 2019
Partial oxidation of methane to methanol by isolated Pt catalyst supported on a CeO 2 nanoparticle journal February 2020

Figures / Tables (9)

Fig. 1(p. 4)figure Fig. 1
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FIG. 5(p. 7)figure FIG. 5
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FIG. 7(p. 9)figure FIG. 7
FIG. 8(p. 9)figure FIG. 8
FIG. 9(p. 10)figure FIG. 9

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