Impurity Control in Catalyst Design: The Role of Sodium in Promoting and Stabilizing Co and Co2C for Syngas Conversion
Abstract
Abstract The design of supported heterogeneous catalysts requires a detailed understanding of the structure and chemistry of the active surface. Although the chemical components of the active phase, support material, and process feed are typically considered to be the most important factors governing catalyst structure and performance, many common commercial supports contain trace impurities, which can have profound effects on catalyst properties. In this work, we study silica‐supported cobalt‐based catalysts, which are widely used in syngas conversion to value‐added products. Supported metallic Co is a commercial Fischer‐Tropsch catalyst, whereas Co 2 C has shown promise for the direct conversion of syngas to higher oxygenates. This study examines the effects of Na, a commonly detected support impurity and a frequently used promoter, on the structure and reactivity of Co and Co 2 C. We show that trace Na impurities significantly decrease catalyst activity of supported metallic Co, and that high Na concentrations result in Co 2 C formation and a loss in Fischer‐Tropsch activity. However, in Co 2 C catalysts, Na plays an important role in stabilizing the Co 2 C phase, but excess Na decreases catalyst activity. We use in situ X‐ray absorption spectroscopy to study Co 2 C formation andmore »
- Authors:
-
[1];
- Stanford Univ., CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Karlsruhe Inst. of Technology (Germany)
- 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 & Biosciences Division; National Science Foundation (NSF); Stanford Nano Shared Facilities; SUNCAT Center for Interface Science and Catalysis; USDOE
- OSTI Identifier:
- 1767931
- Alternate Identifier(s):
- OSTI ID: 1804540
- Grant/Contract Number:
- AC02-76SF00515; ECCS-1542152
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 4; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Cobalt; Cobalt Carbide; EXAFS Spectroscopy; Impurity Effects; Syngas Conversion
Citation Formats
Asundi, Arun S., Hoffman, Adam S., Nathan, Sindhu S., Boubnov, Alexey, Bare, Simon R., and Bent, Stacey F. Impurity Control in Catalyst Design: The Role of Sodium in Promoting and Stabilizing Co and Co2C for Syngas Conversion. United States: N. p., 2021.
Web. doi:10.1002/cctc.202001703.
Asundi, Arun S., Hoffman, Adam S., Nathan, Sindhu S., Boubnov, Alexey, Bare, Simon R., & Bent, Stacey F. Impurity Control in Catalyst Design: The Role of Sodium in Promoting and Stabilizing Co and Co2C for Syngas Conversion. United States. https://doi.org/10.1002/cctc.202001703
Asundi, Arun S., Hoffman, Adam S., Nathan, Sindhu S., Boubnov, Alexey, Bare, Simon R., and Bent, Stacey F. Mon .
"Impurity Control in Catalyst Design: The Role of Sodium in Promoting and Stabilizing Co and Co2C for Syngas Conversion". United States. https://doi.org/10.1002/cctc.202001703. https://www.osti.gov/servlets/purl/1767931.
@article{osti_1767931,
title = {Impurity Control in Catalyst Design: The Role of Sodium in Promoting and Stabilizing Co and Co2C for Syngas Conversion},
author = {Asundi, Arun S. and Hoffman, Adam S. and Nathan, Sindhu S. and Boubnov, Alexey and Bare, Simon R. and Bent, Stacey F.},
abstractNote = {Abstract The design of supported heterogeneous catalysts requires a detailed understanding of the structure and chemistry of the active surface. Although the chemical components of the active phase, support material, and process feed are typically considered to be the most important factors governing catalyst structure and performance, many common commercial supports contain trace impurities, which can have profound effects on catalyst properties. In this work, we study silica‐supported cobalt‐based catalysts, which are widely used in syngas conversion to value‐added products. Supported metallic Co is a commercial Fischer‐Tropsch catalyst, whereas Co 2 C has shown promise for the direct conversion of syngas to higher oxygenates. This study examines the effects of Na, a commonly detected support impurity and a frequently used promoter, on the structure and reactivity of Co and Co 2 C. We show that trace Na impurities significantly decrease catalyst activity of supported metallic Co, and that high Na concentrations result in Co 2 C formation and a loss in Fischer‐Tropsch activity. However, in Co 2 C catalysts, Na plays an important role in stabilizing the Co 2 C phase, but excess Na decreases catalyst activity. We use in situ X‐ray absorption spectroscopy to study Co 2 C formation and decomposition in the Na‐free catalyst under carburization and reaction conditions. The work reveals the importance of carefully controlling alkali metal content, particularly at trace levels, in catalyst design.},
doi = {10.1002/cctc.202001703},
journal = {ChemCatChem},
number = 4,
volume = 13,
place = {United States},
year = {Mon Nov 29 00:00:00 EST 2021},
month = {Mon Nov 29 00:00:00 EST 2021}
}
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