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Title: Synergistic Catalysis between Pd and Fe in Gas Phase Hydrodeoxygenation of m-Cresol

Abstract

Here, a series of Pd/Fe2O3 catalysts were synthesized, characterized, and evaluated for the hydrodeoxygenation (HDO) of m-cresol. It was found that the addition of Pd remarkably promotes the catalytic activity of Fe while the product distributions resemble that of monometallic Fe catalyst, showing high selectivity toward the production of toluene (C–O cleavage without saturation of aromatic ring and C–C cleavage). Reduced catalysts featured with Pd patches on the top of reduced Fe nanoparticle surface, and the interaction between Pd and Fe, was further confirmed using X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy (STEM), and X-ray absorption near edge fine structure (XANES). A possible mechanism, including Pd assisted H2 dissociation and Pd facilitated stabilization of the metallic Fe surface as well as Pd enhanced product desorption, is proposed to be responsible for the high activity and HDO selectivity in Pd–Fe catalysts. The synergic catalysis derived from Pd–Fe interaction found in this work was proved to be applicable to other precious metal promoted Fe catalysts, providing a promising strategy for future design of highly active and selective HDO catalysts.

Authors:
 [1];  [2];  [2];  [3];  [2];  [3];  [3];  [2];  [1]
  1. Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Washington State Univ., Pullman, WA (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Univ. of Delaware, Newark, DE (United States). Synchrotron Catalysis Consortium (SCC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1773667
Grant/Contract Number:  
FG02-05ER15688
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 4; Journal Issue: 10; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 74 ATOMIC AND MOLECULAR PHYSICS; 97 MATHEMATICS AND COMPUTING; hydrodeoxygenation; biomass conversion; bimetallic catalysis; synergistic effects; iron catalyst; noble metal catalysis; H2 sticking

Citation Formats

Hong, Yongchun, Zhang, He, Sun, Junming, Ayman, Karim M., Hensley, Alyssa R., Gu, Meng, Engelhard, Mark H., McEwen, Jean-Sabin, and Wang, Yong. Synergistic Catalysis between Pd and Fe in Gas Phase Hydrodeoxygenation of m-Cresol. United States: N. p., 2014. Web. doi:10.1021/cs500578g.
Hong, Yongchun, Zhang, He, Sun, Junming, Ayman, Karim M., Hensley, Alyssa R., Gu, Meng, Engelhard, Mark H., McEwen, Jean-Sabin, & Wang, Yong. Synergistic Catalysis between Pd and Fe in Gas Phase Hydrodeoxygenation of m-Cresol. United States. https://doi.org/10.1021/cs500578g
Hong, Yongchun, Zhang, He, Sun, Junming, Ayman, Karim M., Hensley, Alyssa R., Gu, Meng, Engelhard, Mark H., McEwen, Jean-Sabin, and Wang, Yong. Tue . "Synergistic Catalysis between Pd and Fe in Gas Phase Hydrodeoxygenation of m-Cresol". United States. https://doi.org/10.1021/cs500578g. https://www.osti.gov/servlets/purl/1773667.
@article{osti_1773667,
title = {Synergistic Catalysis between Pd and Fe in Gas Phase Hydrodeoxygenation of m-Cresol},
author = {Hong, Yongchun and Zhang, He and Sun, Junming and Ayman, Karim M. and Hensley, Alyssa R. and Gu, Meng and Engelhard, Mark H. and McEwen, Jean-Sabin and Wang, Yong},
abstractNote = {Here, a series of Pd/Fe2O3 catalysts were synthesized, characterized, and evaluated for the hydrodeoxygenation (HDO) of m-cresol. It was found that the addition of Pd remarkably promotes the catalytic activity of Fe while the product distributions resemble that of monometallic Fe catalyst, showing high selectivity toward the production of toluene (C–O cleavage without saturation of aromatic ring and C–C cleavage). Reduced catalysts featured with Pd patches on the top of reduced Fe nanoparticle surface, and the interaction between Pd and Fe, was further confirmed using X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy (STEM), and X-ray absorption near edge fine structure (XANES). A possible mechanism, including Pd assisted H2 dissociation and Pd facilitated stabilization of the metallic Fe surface as well as Pd enhanced product desorption, is proposed to be responsible for the high activity and HDO selectivity in Pd–Fe catalysts. The synergic catalysis derived from Pd–Fe interaction found in this work was proved to be applicable to other precious metal promoted Fe catalysts, providing a promising strategy for future design of highly active and selective HDO catalysts.},
doi = {10.1021/cs500578g},
journal = {ACS Catalysis},
number = 10,
volume = 4,
place = {United States},
year = {Tue Jul 29 00:00:00 EDT 2014},
month = {Tue Jul 29 00:00:00 EDT 2014}
}

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