skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Platinum vs transition metal carbide surfaces as catalysts for olefin and alkyne conversion: binding and hydrogenation of ethylidyne

Abstract

The development of heterogeneous catalysts with activity for the hydrogenation of unsaturated hydrocarbons is of economic importance. Ethylene (C 2H 4) and acetylene (C 2H 2) are probe molecules useful to understand the hydrogenation mechanisms, where the most studied surfaces are Pt(111) and Pd(111), however, they have a limited activity due to the formation and accumulation of ethylidyne (CCH 3) species. Therefore, alternative catalysts should be developed to limit and/or avoid the formation of ethylidyne on the surface. Transition metal carbides has been reported as alternative catalysts, with the additional advantage of lower prices. The thermodynamics of ethylidyne binding and its transformations on δ-MoC(001), TiC(001), and β-Mo 2C(100) surfaces are studied by means of periodic DFT. The results indicate that ethylidyne could be transformed to ethyl and ethane on δ-MoC(001) and TiC(001) surfaces, which are relevant species to the Horiuti-Polanyi mechanism. Therefore, these surfaces could be an alternative to Pt(111) and Pd(111), since ethylidyne could be transformed to other species, avoiding or limiting their deactivation. Conversely, ethylidyne cannot be transformed to vinyl (CHCH 2) or ethylene in a Horiuti-Polanyi-like mechanism; then, it is not thermodynamically feasible to use any of the studied surfaces in the selective hydrogenation of acetylene, sincemore » ethylidyne accumulation could poison the surfaces.« less

Authors:
 [1];  [2];  [3]; ORCiD logo [4]
  1. Univ. de Antioquia UdeA, Medellín (Colombia); Univ. de Medellín, Medellín (Colombia)
  2. Univ. de Medellín, Medellín (Colombia)
  3. Univ. de Antioquia UdeA, Medellín (Colombia)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1529882
Report Number(s):
BNL-211802-2019-JAAM
Journal ID: ISSN 1742-6588
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics. Conference Series
Additional Journal Information:
Journal Volume: 1247; Journal ID: ISSN 1742-6588
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Jimenez-Orozco, C., Florez, E., Moreno, A., and Rodriguez, J. A. Platinum vs transition metal carbide surfaces as catalysts for olefin and alkyne conversion: binding and hydrogenation of ethylidyne. United States: N. p., 2019. Web. doi:10.1088/1742-6596/1247/1/012003.
Jimenez-Orozco, C., Florez, E., Moreno, A., & Rodriguez, J. A. Platinum vs transition metal carbide surfaces as catalysts for olefin and alkyne conversion: binding and hydrogenation of ethylidyne. United States. doi:10.1088/1742-6596/1247/1/012003.
Jimenez-Orozco, C., Florez, E., Moreno, A., and Rodriguez, J. A. Sat . "Platinum vs transition metal carbide surfaces as catalysts for olefin and alkyne conversion: binding and hydrogenation of ethylidyne". United States. doi:10.1088/1742-6596/1247/1/012003. https://www.osti.gov/servlets/purl/1529882.
@article{osti_1529882,
title = {Platinum vs transition metal carbide surfaces as catalysts for olefin and alkyne conversion: binding and hydrogenation of ethylidyne},
author = {Jimenez-Orozco, C. and Florez, E. and Moreno, A. and Rodriguez, J. A.},
abstractNote = {The development of heterogeneous catalysts with activity for the hydrogenation of unsaturated hydrocarbons is of economic importance. Ethylene (C2H4) and acetylene (C2H2) are probe molecules useful to understand the hydrogenation mechanisms, where the most studied surfaces are Pt(111) and Pd(111), however, they have a limited activity due to the formation and accumulation of ethylidyne (CCH3) species. Therefore, alternative catalysts should be developed to limit and/or avoid the formation of ethylidyne on the surface. Transition metal carbides has been reported as alternative catalysts, with the additional advantage of lower prices. The thermodynamics of ethylidyne binding and its transformations on δ-MoC(001), TiC(001), and β-Mo2C(100) surfaces are studied by means of periodic DFT. The results indicate that ethylidyne could be transformed to ethyl and ethane on δ-MoC(001) and TiC(001) surfaces, which are relevant species to the Horiuti-Polanyi mechanism. Therefore, these surfaces could be an alternative to Pt(111) and Pd(111), since ethylidyne could be transformed to other species, avoiding or limiting their deactivation. Conversely, ethylidyne cannot be transformed to vinyl (CHCH2) or ethylene in a Horiuti-Polanyi-like mechanism; then, it is not thermodynamically feasible to use any of the studied surfaces in the selective hydrogenation of acetylene, since ethylidyne accumulation could poison the surfaces.},
doi = {10.1088/1742-6596/1247/1/012003},
journal = {Journal of Physics. Conference Series},
number = ,
volume = 1247,
place = {United States},
year = {2019},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Save / Share: