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Title: Elementary Steps of Syngas Reactions on Mo2C(001): Adsorption Thermochemistry and Bond Dissociation

Abstract

Density functional theory (DFT) and ab initio thermodynamics are applied in order to investigate the most stable surface and subsurface terminations of Mo{sub 2}C(001) as a function of chemical potential and in the presence of syngas. The Mo-terminated (001) surface is then used as a model surface to evaluate the thermochemistry and energetic barriers for key elementary steps in syngas reactions. Adsorption energy scaling relations and Broensted-Evans-Polanyi relationships are established and used to place Mo{sub 2}C into the context of transition metal surfaces. The results indicate that the surface termination is a complex function of reaction conditions and kinetics. It is predicted that the surface will be covered by either C{sub 2}H{sub 2} or O depending on conditions. Comparisons to transition metals indicate that the Mo-terminated Mo{sub 2}C(001) surface exhibits carbon reactivity similar to transition metals such as Ru and Ir, but is significantly more reactive towards oxygen.

Authors:
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1035091
Report Number(s):
SLAC-PUB-14660
Journal ID: ISSN 0021-9517; TRN: US201204%%325
DOE Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article
Journal Name:
Submitted to Journal of Catalysis
Additional Journal Information:
Journal Volume: 290; Journal ID: ISSN 0021-9517
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; ADSORPTION; CARBIDES; CARBON; CATALYSIS; DISSOCIATION; DENSITY FUNCTIONAL METHOD; KINETICS; OXYGEN; SYNTHESIS GAS; THERMODYNAMICS; TRANSITION ELEMENTS; CHEM, COMP, MATSCI

Citation Formats

Medford, Andrew. Elementary Steps of Syngas Reactions on Mo2C(001): Adsorption Thermochemistry and Bond Dissociation. United States: N. p., 2012. Web. doi:10.1016/j.jcat.2012.03.007.
Medford, Andrew. Elementary Steps of Syngas Reactions on Mo2C(001): Adsorption Thermochemistry and Bond Dissociation. United States. doi:10.1016/j.jcat.2012.03.007.
Medford, Andrew. Thu . "Elementary Steps of Syngas Reactions on Mo2C(001): Adsorption Thermochemistry and Bond Dissociation". United States. doi:10.1016/j.jcat.2012.03.007. https://www.osti.gov/servlets/purl/1035091.
@article{osti_1035091,
title = {Elementary Steps of Syngas Reactions on Mo2C(001): Adsorption Thermochemistry and Bond Dissociation},
author = {Medford, Andrew},
abstractNote = {Density functional theory (DFT) and ab initio thermodynamics are applied in order to investigate the most stable surface and subsurface terminations of Mo{sub 2}C(001) as a function of chemical potential and in the presence of syngas. The Mo-terminated (001) surface is then used as a model surface to evaluate the thermochemistry and energetic barriers for key elementary steps in syngas reactions. Adsorption energy scaling relations and Broensted-Evans-Polanyi relationships are established and used to place Mo{sub 2}C into the context of transition metal surfaces. The results indicate that the surface termination is a complex function of reaction conditions and kinetics. It is predicted that the surface will be covered by either C{sub 2}H{sub 2} or O depending on conditions. Comparisons to transition metals indicate that the Mo-terminated Mo{sub 2}C(001) surface exhibits carbon reactivity similar to transition metals such as Ru and Ir, but is significantly more reactive towards oxygen.},
doi = {10.1016/j.jcat.2012.03.007},
journal = {Submitted to Journal of Catalysis},
issn = {0021-9517},
number = ,
volume = 290,
place = {United States},
year = {2012},
month = {2}
}