Adsorption and oxidation of propane and cyclopropane on IrO2(110)

Martin, Rachel; Kim, Minkyu; Franklin, Austin; Bian, Yingxue; Asthagiri, Aravind; Weaver, Jason F.

doi:10.1039/c8cp06125d

Title: Adsorption and oxidation of propane and cyclopropane on IrO₂(110)

Abstract

Here, we investigated the adsorption and oxidation of n-propane and cyclopropane (C₃H₈ and c-C₃H₆) on the IrO₂(110) surface using temperature programmed reaction spectroscopy (TPRS) and density functional theory (DFT) calculations. We find that the activation of both C₃H₈ and c-C₃H₆ is facile on IrO₂(110) at low temperature, and that the dissociated alkanes oxidize during TPRS to produce CO, CO₂ and H₂O above ~400 K. Propane conversion to propylene is negligible during TPRS for the conditions studied. Our results show that the maximum yield of alkane that oxidizes during TPRS is higher for c-C₃H₆ compared with C₃H₈ (~0.30 vs. 0.18 monolayer) and that pre-hydrogenation of the surface suppresses c-C₃H₆ oxidation to a lesser extent than C₃H₈. Consistent with the experimental results, DFT predicts that C₃H₈ and c-C₃H₆ form σ-complexes on IrO₂(110) and that C–H bond activation of the complexes as well as subsequent dehydrogenation are highly facile via H-transfer to O_br atoms (bridging O-atoms). Our calculations predict that propane conversion to gaseous propylene is kinetically disfavored on IrO₂(110) because HO_br recombination makes Obr atoms available to promote further dehydrogenation at lower temperatures than those needed for the adsorbed C₃H₆ intermediate to desorb as propylene. We also present evidence that that themore »« less

Authors:

Martin, Rachel ^[1]; Kim, Minkyu ^[2]; Franklin, Austin ^[1]; Bian, Yingxue ^[1]; Asthagiri, Aravind ^[2];

^[1]

Univ. of Florida, Gainesville, FL (United States)
The Ohio State Univ., Columbus, OH (United States)

Publication Date:: Thu Nov 08 00:00:00 EST 2018

Research Org.:: Univ. of Florida, Gainesville, FL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1609450

Alternate Identifier(s):: OSTI ID: 1482258

Grant/Contract Number:: FG02-03ER15478

Resource Type:: Accepted Manuscript

Journal Name:: Physical Chemistry Chemical Physics. PCCP

Additional Journal Information:: Journal Volume: 20; Journal Issue: 46; Journal ID: ISSN 1463-9076

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Physics

Citation Formats


                    Martin, Rachel, Kim, Minkyu, Franklin, Austin, Bian, Yingxue, Asthagiri, Aravind, and Weaver, Jason F. Adsorption and oxidation of propane and cyclopropane on IrO2(110).  United States: N. p., 2018. 
Web.  doi:10.1039/c8cp06125d.

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                    Martin, Rachel, Kim, Minkyu, Franklin, Austin, Bian, Yingxue, Asthagiri, Aravind, & Weaver, Jason F. Adsorption and oxidation of propane and cyclopropane on IrO2(110).  United States.  https://doi.org/10.1039/c8cp06125d

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                    Martin, Rachel, Kim, Minkyu, Franklin, Austin, Bian, Yingxue, Asthagiri, Aravind, and Weaver, Jason F. Thu .  
"Adsorption and oxidation of propane and cyclopropane on IrO2(110)".  United States.  https://doi.org/10.1039/c8cp06125d.  https://www.osti.gov/servlets/purl/1609450.

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@article{osti_1609450,

  title        = {Adsorption and oxidation of propane and cyclopropane on IrO2(110)},

  author       = {Martin, Rachel and Kim, Minkyu and Franklin, Austin and Bian, Yingxue and Asthagiri, Aravind and Weaver, Jason F.},

  abstractNote = {Here, we investigated the adsorption and oxidation of n-propane and cyclopropane (C3H8 and c-C3H6) on the IrO2(110) surface using temperature programmed reaction spectroscopy (TPRS) and density functional theory (DFT) calculations. We find that the activation of both C3H8 and c-C3H6 is facile on IrO2(110) at low temperature, and that the dissociated alkanes oxidize during TPRS to produce CO, CO2 and H2O above ~400 K. Propane conversion to propylene is negligible during TPRS for the conditions studied. Our results show that the maximum yield of alkane that oxidizes during TPRS is higher for c-C3H6 compared with C3H8 (~0.30 vs. 0.18 monolayer) and that pre-hydrogenation of the surface suppresses c-C3H6 oxidation to a lesser extent than C3H8. Consistent with the experimental results, DFT predicts that C3H8 and c-C3H6 form σ-complexes on IrO2(110) and that C–H bond activation of the complexes as well as subsequent dehydrogenation are highly facile via H-transfer to Obr atoms (bridging O-atoms). Our calculations predict that propane conversion to gaseous propylene is kinetically disfavored on IrO2(110) because HObr recombination makes Obr atoms available to promote further dehydrogenation at lower temperatures than those needed for the adsorbed C3H6 intermediate to desorb as propylene. We also present evidence that that the ability for c-C3H6 to activate via ring-opening is responsible for cyclopropane attaining higher reaction yields during TPRS and exhibiting a weaker sensitivity to surface pre-hydrogenation compared with n-propane.},

  doi          = {10.1039/c8cp06125d},

  journal      = {Physical Chemistry Chemical Physics. PCCP},

  number       = 46,

  volume       = 20,

  place        = {United States},

  year         = {Thu Nov 08 00:00:00 EST 2018},

  month        = {Thu Nov 08 00:00:00 EST 2018}

}

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Works referencing / citing this record:

Structure and reactivity of iridium oxide layers grown on Ir(1 0 0) by oxidation at sub-ambient O ₂ pressures
journal, August 2019

Bian, Yingxue; Li, Tao; Weaver, Jason F.
Journal of Physics D: Applied Physics, Vol. 52, Issue 43
DOI: 10.1088/1361-6463/ab32cc

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Title: Adsorption and oxidation of propane and cyclopropane on IrO2(110)

Abstract

Citation Formats

Oxidative dehydrogenation of ethane and propane: How far from commercial implementation? journal, September 2007

Oxidative dehydrogenation of ethane to ethylene over alumina-supported vanadium oxide catalysts: Relationship between molecular structures and chemical reactivity journal, December 2006

Pathways for C–H bond cleavage of propane σ-complexes on PdO(101) journal, January 2012

Dissociative Chemisorption and Oxidation of H2 on the Stoichiometric IrO2(110) Surface journal, December 2017

Generalized Gradient Approximation Made Simple journal, October 1996

Ethane Oxidative Dehydrogenation Pathways on Vanadium Oxide Catalysts journal, May 2002

Projector augmented-wave method journal, December 1994

n-alkanes on Pt(111) and on C(0001)∕Pt(111): Chain length dependence of kinetic desorption parameters journal, December 2006

Oxidative Dehydrogenation of Ethane on Dynamically Rearranging Supported Chloride Catalysts journal, August 2014

Ab initio Hellmann-Feynman molecular dynamics for liquid metals journal, May 1993

Facile Dehydrogenation of Ethane on the IrO 2 (110) Surface journal, February 2018

Ab initio molecular dynamics for liquid metals journal, December 1995

Critical Literature Review of the Kinetics for the Oxidative Dehydrogenation of Propane over Well-Defined Supported Vanadium Oxide Catalysts journal, September 2014

Adsorption of alkanes on stoichiometric and oxygen-rich RuO 2 (110) journal, January 2016

Adsorption of small hydrocarbons on rutile TiO2(110) journal, August 2016

Propane σ-Complexes on PdO(101): Spectroscopic Evidence of the Selective Coordination and Activation of Primary CH Bonds journal, September 2015

Oxidative Dehydrogenation of Ethane: Common Principles and Mechanistic Aspects journal, March 2013

Size-Dependent Catalytic Activity of Supported Vanadium Oxide Species: Oxidative Dehydrogenation of Propane journal, May 2014

A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal, December 2000

Adsorption and Oxidation of n -Butane on the Stoichiometric RuO 2 (110) Surface journal, April 2016

Low-temperature activation of methane on the IrO 2 (110) surface journal, April 2017

Unique Electronic and Structural Effects in Vanadia/Ceria-Catalyzed Reactions journal, October 2015

Supported metal oxide and other catalysts for ethane conversion: a review journal, June 1999

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal, April 2010

Dispersion-corrected density functional theory calculations of the molecular binding of n -alkanes on Pd(111) and PdO(101) journal, February 2012

Effect of Catalyst Structure on Oxidative Dehydrogenation of Ethane and Propane on Alumina-Supported Vanadia journal, May 2002

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Title: Adsorption and oxidation of propane and cyclopropane on IrO₂(110)

Oxidative dehydrogenation of ethane and propane: How far from commercial implementation?
journal, September 2007

Oxidative dehydrogenation of ethane to ethylene over alumina-supported vanadium oxide catalysts: Relationship between molecular structures and chemical reactivity
journal, December 2006

Pathways for C–H bond cleavage of propane σ-complexes on PdO(101)
journal, January 2012

Dissociative Chemisorption and Oxidation of H2 on the Stoichiometric IrO2(110) Surface
journal, December 2017

Generalized Gradient Approximation Made Simple
journal, October 1996

Ethane Oxidative Dehydrogenation Pathways on Vanadium Oxide Catalysts
journal, May 2002

Projector augmented-wave method
journal, December 1994

n-alkanes on Pt(111) and on C(0001)∕Pt(111): Chain length dependence of kinetic desorption parameters
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Oxidative Dehydrogenation of Ethane on Dynamically Rearranging Supported Chloride Catalysts
journal, August 2014

Ab initio Hellmann-Feynman molecular dynamics for liquid metals
journal, May 1993

Facile Dehydrogenation of Ethane on the IrO ₂ (110) Surface
journal, February 2018

Ab initio molecular dynamics for liquid metals
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Critical Literature Review of the Kinetics for the Oxidative Dehydrogenation of Propane over Well-Defined Supported Vanadium Oxide Catalysts
journal, September 2014

Adsorption of alkanes on stoichiometric and oxygen-rich RuO ₂ (110)
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Propane σ-Complexes on PdO(101): Spectroscopic Evidence of the Selective Coordination and Activation of Primary CH Bonds
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Oxidative Dehydrogenation of Ethane: Common Principles and Mechanistic Aspects
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journal, May 2014

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Low-temperature activation of methane on the IrO ₂ (110) surface
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Supported metal oxide and other catalysts for ethane conversion: a review
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A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
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Dispersion-corrected density functional theory calculations of the molecular binding of n -alkanes on Pd(111) and PdO(101)
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