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Title: Effect of carbon supports on RhRe bifunctional catalysts for selective hydrogenolysis of tetrahydropyran-2-methanol

Abstract

Tetrahydropyran-2-methanol undergoes selective C–O–C hydrogenolysis to produce 1,6-hexanediol using a bifunctional RhRe (reducible metal with an oxophilic promoter) catalyst supported on Vulcan XC-72 carbon (VXC) with >90% selectivity. This RhRe/VXC catalyst is stable over 40 h of reaction in a continuous flow fixed bed reactor. The hydrogenolysis activity of RhRe/VXC is two orders-of-magnitude higher than that of RhRe supported on Norit Darco 12X40 activated carbon (NDC). STEM–EDS analysis reveals that, compared to the RhRe/VXC catalyst, the Re and Rh component metals are segregated on the surface of the low activity RhRe/NDC catalyst, suggesting that Rh and Re in close proximity (“bimetallic” particles) are required for an active hydrogenolysis catalyst. Differences in metal distribution on the carbon surfaces are, in turn, linked to the properties of the carbons: NDC has both a higher surface area and surface oxygen content. Thus, the low areal density of Rh and Re precursors on the high area NDC and/or interactions of the precursors with its O functional groups may interfere with the formation of the bimetallic species required for an active catalyst.

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [3];  [1];  [4];  [1];  [1]
  1. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering
  2. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering; Northeast Normal Univ., Changchun (China). Dept. of Chemistry and Key Lab. of Polyoxometalate Science of the Ministry Education
  3. Northeast Normal Univ., Changchun (China). Dept. of Chemistry and Key Lab. of Polyoxometalate Science of the Ministry Education
  4. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering and Dept. of Chemistry
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Canadian Light Sources, Inc., Saskatoon, SK (Canada); National Science Foundation (NSF); China Scholarship Council (CSC)
OSTI Identifier:
1438096
Grant/Contract Number:  
EE0006878; AC02-06CH11357; DMR-1121288; DMR-0832760
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Catalysis Science and Technology
Additional Journal Information:
Journal Volume: 6; Journal Issue: 21; Journal ID: ISSN 2044-4753
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 09 BIOMASS FUELS

Citation Formats

Karanjkar, Pranav U., Burt, Samuel P., Chen, Xiaoli, Barnett, Kevin J., Ball, Madelyn R., Kumbhalkar, Mrunmayi D., Wang, Xiaohong, Miller, James B., Hermans, Ive, Dumesic, James A., and Huber, George W. Effect of carbon supports on RhRe bifunctional catalysts for selective hydrogenolysis of tetrahydropyran-2-methanol. United States: N. p., 2016. Web. doi:10.1039/c6cy01763k.
Karanjkar, Pranav U., Burt, Samuel P., Chen, Xiaoli, Barnett, Kevin J., Ball, Madelyn R., Kumbhalkar, Mrunmayi D., Wang, Xiaohong, Miller, James B., Hermans, Ive, Dumesic, James A., & Huber, George W. Effect of carbon supports on RhRe bifunctional catalysts for selective hydrogenolysis of tetrahydropyran-2-methanol. United States. doi:10.1039/c6cy01763k.
Karanjkar, Pranav U., Burt, Samuel P., Chen, Xiaoli, Barnett, Kevin J., Ball, Madelyn R., Kumbhalkar, Mrunmayi D., Wang, Xiaohong, Miller, James B., Hermans, Ive, Dumesic, James A., and Huber, George W. Mon . "Effect of carbon supports on RhRe bifunctional catalysts for selective hydrogenolysis of tetrahydropyran-2-methanol". United States. doi:10.1039/c6cy01763k. https://www.osti.gov/servlets/purl/1438096.
@article{osti_1438096,
title = {Effect of carbon supports on RhRe bifunctional catalysts for selective hydrogenolysis of tetrahydropyran-2-methanol},
author = {Karanjkar, Pranav U. and Burt, Samuel P. and Chen, Xiaoli and Barnett, Kevin J. and Ball, Madelyn R. and Kumbhalkar, Mrunmayi D. and Wang, Xiaohong and Miller, James B. and Hermans, Ive and Dumesic, James A. and Huber, George W.},
abstractNote = {Tetrahydropyran-2-methanol undergoes selective C–O–C hydrogenolysis to produce 1,6-hexanediol using a bifunctional RhRe (reducible metal with an oxophilic promoter) catalyst supported on Vulcan XC-72 carbon (VXC) with >90% selectivity. This RhRe/VXC catalyst is stable over 40 h of reaction in a continuous flow fixed bed reactor. The hydrogenolysis activity of RhRe/VXC is two orders-of-magnitude higher than that of RhRe supported on Norit Darco 12X40 activated carbon (NDC). STEM–EDS analysis reveals that, compared to the RhRe/VXC catalyst, the Re and Rh component metals are segregated on the surface of the low activity RhRe/NDC catalyst, suggesting that Rh and Re in close proximity (“bimetallic” particles) are required for an active hydrogenolysis catalyst. Differences in metal distribution on the carbon surfaces are, in turn, linked to the properties of the carbons: NDC has both a higher surface area and surface oxygen content. Thus, the low areal density of Rh and Re precursors on the high area NDC and/or interactions of the precursors with its O functional groups may interfere with the formation of the bimetallic species required for an active catalyst.},
doi = {10.1039/c6cy01763k},
journal = {Catalysis Science and Technology},
issn = {2044-4753},
number = 21,
volume = 6,
place = {United States},
year = {2016},
month = {9}
}

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Works referenced in this record:

Aqueous Phase Glycerol Reforming by PtMo Bimetallic Nano-Particle Catalyst: Product Selectivity and Structural Characterization
journal, February 2012

  • Dietrich, Paul J.; Lobo-Lapidus, Rodrigo J.; Wu, Tianpin
  • Topics in Catalysis, Vol. 55, Issue 1-2, p. 53-69
  • DOI: 10.1007/s11244-012-9775-5