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Title: Modeling the Adsorbate Coverage Distribution Over a Multi-Faceted Catalytic Grain in the Presence of an Electric Field: O/Fe from First Principles

Abstract

The impact of an external electric field on the concerted behavior of oxygen over a multi-faceted catalytic Fe grain is determined via the interpolation of ab initio models of oxygen adsorption on Fe(100), Fe(110), and Fe(111) in the presence of an external electric field. The application of both negative and positive electric fields weaken the adsorption strength for oxygen on all three surface facets, with Fe(110) experiencing the greatest effect. Kinetic models of a multi-faceted catalytic Fe grain show that the average oxygen coverage over the grain surface is reduced under the influence of both a negative and positive electric field, which are consistent with phase diagram results at comparable pressures. Furthermore, we show that there is a weak synergistic effect between a Pd promoter and a positive electric field on the oxygen adsorption energy, i.e. the Pd promoter and electric field combination weaken the oxygen adsorption energy to a greater degree than the simple addition of both components separately. In conclusion, the work shows that the application of an applied external electric field may be a useful tool in fine-tuning chemical properties of Fe-based catalysts in hydrodeoxygenation applications.

Authors:
 [1];  [1];  [1];  [1];  [2];  [3]
  1. Washington State Univ., Pullman, WA (United States). The Gene and Linda Voiland School of Chemical Engineering and Bioengineering
  2. Washington State Univ., Pullman, WA (United States). The Gene and Linda Voiland School of Chemical Engineering and Bioengineering and Dept. of Chemistry; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis
  3. Washington State Univ., Pullman, WA (United States). The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Dept. of Chemistry, Dept. of Physics and Astronomy and Dept. of Biological Systems Engineering; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; Washington State Univ., Pullman, WA (United States); Achievement Rewards for College Scientists Foundation, Inc. (ARCS); USDOE
OSTI Identifier:
1434659
Alternate Identifier(s):
OSTI ID: 1591659
Report Number(s):
PNNL-SA-138082
Journal ID: ISSN 0920-5861; PII: S0920586118304188
Grant/Contract Number:  
SC0014560; AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 312; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 09 BIOMASS FUELS; Field ion microscopy; Heterogeneous catalysis; Iron; Oxygen; Hydrodeoxygenation; Mean Field Model

Citation Formats

Bray, Jacob, Hensley, Alyssa J. R., Collinge, Greg, Che, Fanglin, Wang, Yong, and McEwen, Jean-Sabin. Modeling the Adsorbate Coverage Distribution Over a Multi-Faceted Catalytic Grain in the Presence of an Electric Field: O/Fe from First Principles. United States: N. p., 2018. Web. doi:10.1016/J.CATTOD.2018.04.016.
Bray, Jacob, Hensley, Alyssa J. R., Collinge, Greg, Che, Fanglin, Wang, Yong, & McEwen, Jean-Sabin. Modeling the Adsorbate Coverage Distribution Over a Multi-Faceted Catalytic Grain in the Presence of an Electric Field: O/Fe from First Principles. United States. doi:10.1016/J.CATTOD.2018.04.016.
Bray, Jacob, Hensley, Alyssa J. R., Collinge, Greg, Che, Fanglin, Wang, Yong, and McEwen, Jean-Sabin. Sun . "Modeling the Adsorbate Coverage Distribution Over a Multi-Faceted Catalytic Grain in the Presence of an Electric Field: O/Fe from First Principles". United States. doi:10.1016/J.CATTOD.2018.04.016. https://www.osti.gov/servlets/purl/1434659.
@article{osti_1434659,
title = {Modeling the Adsorbate Coverage Distribution Over a Multi-Faceted Catalytic Grain in the Presence of an Electric Field: O/Fe from First Principles},
author = {Bray, Jacob and Hensley, Alyssa J. R. and Collinge, Greg and Che, Fanglin and Wang, Yong and McEwen, Jean-Sabin},
abstractNote = {The impact of an external electric field on the concerted behavior of oxygen over a multi-faceted catalytic Fe grain is determined via the interpolation of ab initio models of oxygen adsorption on Fe(100), Fe(110), and Fe(111) in the presence of an external electric field. The application of both negative and positive electric fields weaken the adsorption strength for oxygen on all three surface facets, with Fe(110) experiencing the greatest effect. Kinetic models of a multi-faceted catalytic Fe grain show that the average oxygen coverage over the grain surface is reduced under the influence of both a negative and positive electric field, which are consistent with phase diagram results at comparable pressures. Furthermore, we show that there is a weak synergistic effect between a Pd promoter and a positive electric field on the oxygen adsorption energy, i.e. the Pd promoter and electric field combination weaken the oxygen adsorption energy to a greater degree than the simple addition of both components separately. In conclusion, the work shows that the application of an applied external electric field may be a useful tool in fine-tuning chemical properties of Fe-based catalysts in hydrodeoxygenation applications.},
doi = {10.1016/J.CATTOD.2018.04.016},
journal = {Catalysis Today},
number = ,
volume = 312,
place = {United States},
year = {2018},
month = {4}
}

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