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Title: Sulfur-Tolerant Molybdenum Carbide Catalysts Enabling Low-Temperature Stabilization of Fast Pyrolysis Bio-oil

Low-temperature hydrogenation of carbonyl fractions can greatly improve the thermal stability of fast pyrolysis bio-oil which is crucial to achieve long-term operation of high-temperature upgrading reactors. The current state of the art, precious metals such as ruthenium, although highly effective in carbonyl hydrogenation, rapidly loses performance due to sulfur sensitivity. The present work showed that molybdenum carbides were active and sulfur-tolerant in low-temperature conversion carbonyl compounds. Furthermore, due to surface bifunctionality (presence of both metallic and acid sites), carbides catalyzed both C=O bond hydrogenation and C-C coupling reactions retaining most of carbon atoms in liquid products as more stable and higher molecular weight oligomeric compounds while consuming less hydrogen than ruthenium. The carbides proved to be resistant to other deactivation mechanisms including hydrothermal aging, oxidation, coking and leaching. These properties enabled carbides to achieve and maintain good catalytic performance in both aqueous-phase furfural conversion and real bio-oil stabilization with sulfur present. This finding strongly suggests that molybdenum carbides can provide a catalyst solution necessary for the development of commercially viable bio-oil stabilization technology.
Authors:
 [1] ; ORCiD logo [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Report Number(s):
PNNL-SA-128200
Journal ID: ISSN 0887-0624; BM0108020
Grant/Contract Number:
AC05-76RL01830; AC05-00OR22725
Type:
Published Article
Journal Name:
Energy and Fuels
Additional Journal Information:
Journal Volume: 31; Journal Issue: 9; Journal ID: ISSN 0887-0624
Publisher:
American Chemical Society (ACS)
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); UT-Battelle, LLC, Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 09 BIOMASS FUELS
OSTI Identifier:
1378832
Alternate Identifier(s):
OSTI ID: 1398192; OSTI ID: 1421365