Journal
JOURNAL OF CATALYSIS
Volume 315, Issue -, Pages 48-58Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2014.03.016
Keywords
Hydrogenolysis; Ring opening cyclic ethers; DFT, bifunctional catalysis; Hydrodeoxygenation; Oxophilic metal promoters; Deprotonation energies; Hydroxymethyl tetrahydrofuran
Categories
Funding
- National Science Foundation under the NSF Award, Center for Biorenewable Chemicals (CBiRC) at Iowa State University [EEC-0813570]
- NSF award for the Partnership in International Research and Education (PIRE) [OISE 0730277]
- U.S. Department of Energy, Office of Biological and Environmental Research at the Pacific Northwest National Laboratory
Ask authors/readers for more resources
The promotion of metal catalysts with partially oxidized oxophilic MOx species, such as ReOx-promoted Rh, has been demonstrated to produce Bronsted acid sites that can promote hydrogenolysis of oxygenate intermediates such as those found in biomass-derived species. A wide variety of alloy compositions and structures are examined in this work to investigate strongly acidic promoters by using DFT-calculated deprotonation energies (DPE) as a measure of acid strength. Sites with the highest acid strength had DPE less than 1100 kJ mol(-1), similar to DPE values of heteropolyacids or acid-containing zeolites, and were found on alloys composed of an oxophilic metal (such as Re or W) with a noble metal (such as Rh or Pt). NH3 adsorbs more strongly to sites with increasing acid strength and the activation barriers for acid-catalyzed ring opening of a furan ring decrease with increasing acid strength, which was also shown to be stronger for OH acid sites bound to multiple oxophilic metal atoms in a three-fold configuration rather than OH sites adsorbed in an atop configuration on one oxophilic metal, indicating that small MOx clusters may yield sites with the highest acid strength. (C) 2014 Published by Elsevier Inc.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available