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Title: Structural evolution of molybdenum carbides in hot aqueous environments and impact on low-temperature hydroprocessing of acetic acid

Abstract

In this paper, we investigated the structural evolution of molybdenum carbides subjected to hot aqueous environments and their catalytic performance in low-temperature hydroprocessing of acetic acid. While bulk structures of Mo carbides were maintained after aging in hot liquid water, a portion of carbidic Mo sites were converted to oxidic sites. Water aging also induced changes to the non-carbidic carbon deposited during carbide synthesis and increased surface roughness, which in turn affected carbide pore volume and surface area. The extent of these structural changes was sensitive to the initial carbide structure and was lower under actual hydroprocessing conditions indicating the possibility of further improving the hydrothermal stability of Mo carbides by optimizing catalyst structure and operating conditions. Mo carbides were active in acetic acid conversion in the presence of liquid water, their activity being comparable to that of Ru/C. Finally, the results suggest that effective and inexpensive bio-oil hydroprocessing catalysts could be designed based on Mo carbides, although a more detailed understanding of the structure-performance relationships is needed, especially in upgrading of more complex reaction mixtures or real bio-oils.

Authors:
 [1];  [1];  [2];  [2];  [1];  [1];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Kentucky, Lexington, KY (United States). Center for Applied Energy Research
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Kentucky, Lexington, KY (United States)
OSTI Identifier:
1185780
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Catalysts
Additional Journal Information:
Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2073-4344
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; molybdenum carbide; Mo2C; biomass; bio-oil; pyrolysis oil; hydroprocessing; acetic acid hydrogenation; heterogeneous catalysis

Citation Formats

Choi, Jae -Soon, Schwartz, Viviane, Santillan-Jimenez, Eduardo, Crocker, Mark, Lewis, Sr., Samuel A., Lance, Michael J., Meyer, III, Harry M., and More, Karren L. Structural evolution of molybdenum carbides in hot aqueous environments and impact on low-temperature hydroprocessing of acetic acid. United States: N. p., 2015. Web. doi:10.3390/catal5010406.
Choi, Jae -Soon, Schwartz, Viviane, Santillan-Jimenez, Eduardo, Crocker, Mark, Lewis, Sr., Samuel A., Lance, Michael J., Meyer, III, Harry M., & More, Karren L. Structural evolution of molybdenum carbides in hot aqueous environments and impact on low-temperature hydroprocessing of acetic acid. United States. doi:10.3390/catal5010406.
Choi, Jae -Soon, Schwartz, Viviane, Santillan-Jimenez, Eduardo, Crocker, Mark, Lewis, Sr., Samuel A., Lance, Michael J., Meyer, III, Harry M., and More, Karren L. Fri . "Structural evolution of molybdenum carbides in hot aqueous environments and impact on low-temperature hydroprocessing of acetic acid". United States. doi:10.3390/catal5010406. https://www.osti.gov/servlets/purl/1185780.
@article{osti_1185780,
title = {Structural evolution of molybdenum carbides in hot aqueous environments and impact on low-temperature hydroprocessing of acetic acid},
author = {Choi, Jae -Soon and Schwartz, Viviane and Santillan-Jimenez, Eduardo and Crocker, Mark and Lewis, Sr., Samuel A. and Lance, Michael J. and Meyer, III, Harry M. and More, Karren L.},
abstractNote = {In this paper, we investigated the structural evolution of molybdenum carbides subjected to hot aqueous environments and their catalytic performance in low-temperature hydroprocessing of acetic acid. While bulk structures of Mo carbides were maintained after aging in hot liquid water, a portion of carbidic Mo sites were converted to oxidic sites. Water aging also induced changes to the non-carbidic carbon deposited during carbide synthesis and increased surface roughness, which in turn affected carbide pore volume and surface area. The extent of these structural changes was sensitive to the initial carbide structure and was lower under actual hydroprocessing conditions indicating the possibility of further improving the hydrothermal stability of Mo carbides by optimizing catalyst structure and operating conditions. Mo carbides were active in acetic acid conversion in the presence of liquid water, their activity being comparable to that of Ru/C. Finally, the results suggest that effective and inexpensive bio-oil hydroprocessing catalysts could be designed based on Mo carbides, although a more detailed understanding of the structure-performance relationships is needed, especially in upgrading of more complex reaction mixtures or real bio-oils.},
doi = {10.3390/catal5010406},
journal = {Catalysts},
number = 1,
volume = 5,
place = {United States},
year = {Fri Mar 13 00:00:00 EDT 2015},
month = {Fri Mar 13 00:00:00 EDT 2015}
}

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Cited by: 7 works
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Works referenced in this record:

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