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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. Overall, 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];  [2];  [1];  [2];  [1];  [1]
  1. WASHINGTON STATE UNIV
  2. Washington State University
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1518597
Report Number(s):
PNNL-SA-138082
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 312
Country of Publication:
United States
Language:
English

Citation Formats

Bray, Jacob E., Hensley, Alyssa, Collinge, Gregory B., 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 E., Hensley, Alyssa, Collinge, Gregory B., 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 E., Hensley, Alyssa, Collinge, Gregory B., Che, Fanglin, Wang, Yong, and Mcewen, Jean Sabin. Wed . "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.
@article{osti_1518597,
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 E. and Hensley, Alyssa and Collinge, Gregory B. 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. Overall, 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 = {8}
}