Graphitic mesoporous carbon-supported molybdenum carbides for catalytic hydrogenation of carbon monoxide to mixed alcohols

Song Hai Chai, Viviane Schwartz, Jane Y. Howe, Xiqing Wang, Michelle Kidder, Steven H. Overbury, Sheng Dai, De En Jiang

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27 Scopus citations

Abstract

Molybdenum carbide (β-Mo2C) nanoparticles were synthesized in situ on a soft-templated graphitic mesoporous carbon (GMC) and other commercial carbon materials (activated charcoal and carbon black) by carbothermal hydrogen reduction (i.e., carbon supports as carburizing agents). The catalytic activity of these carbon-supported and bulk carbides for carbon monoxide (CO) hydrogenation to mixed alcohols (mainly C1-C 3) was investigated at 573 K and 3.0 MPa, showing that their areal specific rates for CO conversion increase with decreasing the carbide particle size, independent of the supports. GMC appears to be a preferable support of β-Mo2C to activated charcoal and carbon black because of its ability for the formation of smaller carbide particles resulting in higher catalytic activity. Addition of a minor amount of K2CO3 into β-Mo2C/GMC (molar K/Mo = 0.05-0.5) promotes the formation of higher alcohols (C2+-OH) considerably, leading to a maximum space time yield (STY) for C2+-OH at medium K/Mo ratio of 0.1. Compared with typical Rh/GMC catalyst promoted triply with Mn, Li, and Fe oxides, the K2CO3-promoted β-Mo2C/GMC catalyst shows higher C2+-OH selectivity (30 vs. 25 mol-C% on CO2-free basis) and STY (71 vs. 46 mg (h gcat)-1) in spite of its suppressed formation of CH3OH.

Original languageEnglish
Pages (from-to)141-149
Number of pages9
JournalMicroporous and Mesoporous Materials
Volume170
DOIs
StatePublished - 2013

Funding

This work was supported by the laboratory-directed research and development (LDRD) program of Oak Ridge National Laboratory, managed and operated by UT-Battelle, LLC. A portion of this research was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. Department of Energy. The microscopy work was carried out using ORNL’s Shared Research Equipment (ShaRE) User Facility that sponsored by the Office of Basic Energy Sciences, U.S. Department of Energy. The authors thank the reviewers for their valuable comments and suggestions to considerably improve the quality of this manuscript.

FundersFunder number
U.S. Department of Energy
Basic Energy Sciences
Oak Ridge National Laboratory

    Keywords

    • Alcohol synthesis
    • Heterogeneous catalysis
    • Mesoporous carbon
    • Molybdenum carbides
    • Synthesis gas conversion

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