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Title: Systematic Structure–Property Relationship Studies in Palladium-Catalyzed Methane Complete Combustion

Abstract

To limit further rising levels in methane emissions from stationary and mobile sources and to enable promising technologies based on methane, the development of efficient combustion catalysts that completely oxidize CH4 to CO2 and H2O at low temperatures in the presence of high steam concentrations is required. Palladium is widely considered as one of the most promising materials for this reaction, and a better understanding of the factors affecting its activity and stability is crucial to design even more improved catalysts that efficiently utilize this precious metal. Here we report a study of the effect of three important variables (particle size, support, and reaction conditions including water) on the activity of supported Pd catalysts. We use uniform palladium nanocrystals as catalyst precursors to prepare a library of well-defined catalysts to systematically describe structure–property relationships with help from theory and in situ X-ray absorption spectroscopy. With this approach, we confirm that PdO is the most active phase and that small differences in reaction rates as a function of size are likely due to variations in the surface crystal structure. We further demonstrate that the support exerts a limited influence on the PdO activity, with inert (SiO2), acidic (Al2O3), and redox-active (Ce0.8Zr0.2O2)more » supports providing similar rates, while basic (MgO) supports show remarkably lower activity. Finally, we show that the introduction of steam leads to a considerable decrease in rates that is due to coverage effects, rather than structural and/or phase changes. Altogether, the data suggest that to further increase the activity and stability of Pd-based catalysts for methane combustion, increasing the surface area of supported PdO phases while avoiding strong adsorption of water on the catalytic surfaces is required. This study clarifies contrasting reports in the literature about the active phase and stability of Pd-based materials for methane combustion.« less

Authors:
 [1];  [2];  [3];  [1];  [3];  [1];  [2];  [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1457139
Alternate Identifier(s):
OSTI ID: 1485426
Grant/Contract Number:  
DGE-1656518; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 7; Journal Issue: 11; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; in situ XAS; methane complete combustion; nanocrystals; palladium catalysts; structure−property relationships

Citation Formats

Willis, Joshua J., Gallo, Alessandro, Sokaras, Dimosthenis, Aljama, Hassan, Nowak, Stanislaw H., Goodman, Emmett D., Wu, Liheng, Tassone, Christopher J., Jaramillo, Thomas F., Abild-Pedersen, Frank, and Cargnello, Matteo. Systematic Structure–Property Relationship Studies in Palladium-Catalyzed Methane Complete Combustion. United States: N. p., 2017. Web. doi:10.1021/acscatal.7b02414.
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Willis, Joshua J., Gallo, Alessandro, Sokaras, Dimosthenis, Aljama, Hassan, Nowak, Stanislaw H., Goodman, Emmett D., Wu, Liheng, Tassone, Christopher J., Jaramillo, Thomas F., Abild-Pedersen, Frank, & Cargnello, Matteo. Systematic Structure–Property Relationship Studies in Palladium-Catalyzed Methane Complete Combustion. United States. https://doi.org/10.1021/acscatal.7b02414
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Willis, Joshua J., Gallo, Alessandro, Sokaras, Dimosthenis, Aljama, Hassan, Nowak, Stanislaw H., Goodman, Emmett D., Wu, Liheng, Tassone, Christopher J., Jaramillo, Thomas F., Abild-Pedersen, Frank, and Cargnello, Matteo. Mon . "Systematic Structure–Property Relationship Studies in Palladium-Catalyzed Methane Complete Combustion". United States. https://doi.org/10.1021/acscatal.7b02414. https://www.osti.gov/servlets/purl/1457139.
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@article{osti_1457139,
title = {Systematic Structure–Property Relationship Studies in Palladium-Catalyzed Methane Complete Combustion},
author = {Willis, Joshua J. and Gallo, Alessandro and Sokaras, Dimosthenis and Aljama, Hassan and Nowak, Stanislaw H. and Goodman, Emmett D. and Wu, Liheng and Tassone, Christopher J. and Jaramillo, Thomas F. and Abild-Pedersen, Frank and Cargnello, Matteo},
abstractNote = {To limit further rising levels in methane emissions from stationary and mobile sources and to enable promising technologies based on methane, the development of efficient combustion catalysts that completely oxidize CH4 to CO2 and H2O at low temperatures in the presence of high steam concentrations is required. Palladium is widely considered as one of the most promising materials for this reaction, and a better understanding of the factors affecting its activity and stability is crucial to design even more improved catalysts that efficiently utilize this precious metal. Here we report a study of the effect of three important variables (particle size, support, and reaction conditions including water) on the activity of supported Pd catalysts. We use uniform palladium nanocrystals as catalyst precursors to prepare a library of well-defined catalysts to systematically describe structure–property relationships with help from theory and in situ X-ray absorption spectroscopy. With this approach, we confirm that PdO is the most active phase and that small differences in reaction rates as a function of size are likely due to variations in the surface crystal structure. We further demonstrate that the support exerts a limited influence on the PdO activity, with inert (SiO2), acidic (Al2O3), and redox-active (Ce0.8Zr0.2O2) supports providing similar rates, while basic (MgO) supports show remarkably lower activity. Finally, we show that the introduction of steam leads to a considerable decrease in rates that is due to coverage effects, rather than structural and/or phase changes. Altogether, the data suggest that to further increase the activity and stability of Pd-based catalysts for methane combustion, increasing the surface area of supported PdO phases while avoiding strong adsorption of water on the catalytic surfaces is required. This study clarifies contrasting reports in the literature about the active phase and stability of Pd-based materials for methane combustion.},
doi = {10.1021/acscatal.7b02414},
journal = {ACS Catalysis},
number = 11,
volume = 7,
place = {United States},
year = {2017},
month = {10}
}
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Journal Article:
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https://doi.org/10.1021/acscatal.7b02414
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Cited by: 114 works
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Figures / Tables:

Figure 1 Figure 1: Representative TEM images (A-E), small angle X-ray scattering patterns (F-J), and particle size distributions (K-O) for uniform Pd NCS (from left to right x-small, small, medium, large, and x-large, respectively). For TEM measurements, N ≥ 300 counts.
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