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Title: Unraveling the mechanism of the hydrodeoxygenation of propionic acid over a Pt (1 1 1) surface in vapor and liquid phases

Abstract

Microkinetic models based on first principles calculations have been developed for the vapor and liquid phase hydrodeoxygenation of propionic acid over a Pt (1 1 1) surface. Calculations suggest that decarboxylation does not occur at an appreciable rate. In the vapor phase, decarbonylation products, propanal and propanol are all produced at similar rates. However, in both liquid water and 1,4-dioxane, propanol and propanal are favored over decarbonylation products. While a condensed phase can shift the reaction rate and selectivity significantly, the dominant pathways towards the various products are hardly affected. Only for propanal production do we observe a shift in mechanism. At 473 K, the propionic acid conversion rate is increased by one order of magnitude in liquid 1,4-dioxane relative to the gas phase. In liquid water, the conversion rate is similar to the vapor phase since adsorbed propionic acid blocks a large fraction of the surface sites.

Authors:
 [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. University of South Carolina, Columbia, SC (United States)
  2. Syracuse University, NY (United States)
Publication Date:
Research Org.:
Univ. of South Carolina, Columbia, SC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); USDOE
OSTI Identifier:
1656894
Alternate Identifier(s):
OSTI ID: 1691902
Grant/Contract Number:  
SC0007167; DMREF-1534260; DMREF-1534269; TG-CTS090100
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 381; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Propionic acid; Hydrodeoxygenation mechanism; Propanol; Propionaldehyde; Microkinetic modeling; Solvent effect; Lateral interaction

Citation Formats

Yang, Wenqiang, Solomon, Rajadurai Vijay, Lu, Jianmin, Mamun, Osman, Bond, Jesse Q., and Heyden, Andreas. Unraveling the mechanism of the hydrodeoxygenation of propionic acid over a Pt (1 1 1) surface in vapor and liquid phases. United States: N. p., 2019. Web. https://doi.org/10.1016/j.jcat.2019.11.036.
Yang, Wenqiang, Solomon, Rajadurai Vijay, Lu, Jianmin, Mamun, Osman, Bond, Jesse Q., & Heyden, Andreas. Unraveling the mechanism of the hydrodeoxygenation of propionic acid over a Pt (1 1 1) surface in vapor and liquid phases. United States. https://doi.org/10.1016/j.jcat.2019.11.036
Yang, Wenqiang, Solomon, Rajadurai Vijay, Lu, Jianmin, Mamun, Osman, Bond, Jesse Q., and Heyden, Andreas. Wed . "Unraveling the mechanism of the hydrodeoxygenation of propionic acid over a Pt (1 1 1) surface in vapor and liquid phases". United States. https://doi.org/10.1016/j.jcat.2019.11.036. https://www.osti.gov/servlets/purl/1656894.
@article{osti_1656894,
title = {Unraveling the mechanism of the hydrodeoxygenation of propionic acid over a Pt (1 1 1) surface in vapor and liquid phases},
author = {Yang, Wenqiang and Solomon, Rajadurai Vijay and Lu, Jianmin and Mamun, Osman and Bond, Jesse Q. and Heyden, Andreas},
abstractNote = {Microkinetic models based on first principles calculations have been developed for the vapor and liquid phase hydrodeoxygenation of propionic acid over a Pt (1 1 1) surface. Calculations suggest that decarboxylation does not occur at an appreciable rate. In the vapor phase, decarbonylation products, propanal and propanol are all produced at similar rates. However, in both liquid water and 1,4-dioxane, propanol and propanal are favored over decarbonylation products. While a condensed phase can shift the reaction rate and selectivity significantly, the dominant pathways towards the various products are hardly affected. Only for propanal production do we observe a shift in mechanism. At 473 K, the propionic acid conversion rate is increased by one order of magnitude in liquid 1,4-dioxane relative to the gas phase. In liquid water, the conversion rate is similar to the vapor phase since adsorbed propionic acid blocks a large fraction of the surface sites.},
doi = {10.1016/j.jcat.2019.11.036},
journal = {Journal of Catalysis},
number = ,
volume = 381,
place = {United States},
year = {2019},
month = {12}
}

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