Carboxyl group enhanced CO tolerant GO supported Pt catalysts: DFT and electrochemical analysis

S. Sharma, M. N. Groves, J. Fennell, Navneet Soin, S. L. Horswell, C. Malardier-Jugroot

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Abstract

The effect of residual oxygen species in as-prepared Pt nanoparticle on partially reduced graphene oxide (Pt/PRGO) and partially reduced carboxylated-GO (Pt/PR(GO-COOH)) supports was investigated using electrochemical CO stripping and density functional theory (DFT) analysis. Pt/PRGO and Pt/PR(GO-COOH) revealed a clear negative shift in CO-stripping onset potential compared to commercial Pt/carbon black. DFT analysis confirmed that the presence of a -COOH group provides the most resistance for CO adsorption. This CO-Pt binding energy is significantly lower than that observed in the presence of an OH group, which is the most abundant oxygen group in carbon supports. The Pt-CO dissociation energies (on a 42-atom graphene sheet) in the presence of various oxygen groups, in descending order, were OH > C=O ≈ C-O-C > COOH. Although single-bonded carbon-oxygen groups (-OH and C-O-C) are more abundant on the GO basal plane and play an important role in Pt nanoparticle nucleation and distribution on graphene sheets, the double-bonded carbon-oxygen (C=O and COOH) groups are more abundant residual species post Pt nanoparticle growth and play a vital role in enhancing CO tolerance.

LanguageEnglish
Pages6142-6151
Number of pages10
JournalChemistry of Materials
Volume26
Issue number21
DOIs
Publication statusPublished - 11 Nov 2014

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Carbon Monoxide
Catalyst supports
Density functional theory
Graphite
Graphene
Oxygen
Nanoparticles
Carbon
Oxides
Soot
Carbon black
Binding energy
Nucleation
Adsorption
Atoms

Cite this

Sharma, S., Groves, M. N., Fennell, J., Soin, N., Horswell, S. L., & Malardier-Jugroot, C. (2014). Carboxyl group enhanced CO tolerant GO supported Pt catalysts: DFT and electrochemical analysis. Chemistry of Materials, 26(21), 6142-6151. https://doi.org/10.1021/cm502447s
Sharma, S. ; Groves, M. N. ; Fennell, J. ; Soin, Navneet ; Horswell, S. L. ; Malardier-Jugroot, C. / Carboxyl group enhanced CO tolerant GO supported Pt catalysts : DFT and electrochemical analysis. In: Chemistry of Materials. 2014 ; Vol. 26, No. 21. pp. 6142-6151.
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abstract = "The effect of residual oxygen species in as-prepared Pt nanoparticle on partially reduced graphene oxide (Pt/PRGO) and partially reduced carboxylated-GO (Pt/PR(GO-COOH)) supports was investigated using electrochemical CO stripping and density functional theory (DFT) analysis. Pt/PRGO and Pt/PR(GO-COOH) revealed a clear negative shift in CO-stripping onset potential compared to commercial Pt/carbon black. DFT analysis confirmed that the presence of a -COOH group provides the most resistance for CO adsorption. This CO-Pt binding energy is significantly lower than that observed in the presence of an OH group, which is the most abundant oxygen group in carbon supports. The Pt-CO dissociation energies (on a 42-atom graphene sheet) in the presence of various oxygen groups, in descending order, were OH > C=O ≈ C-O-C > COOH. Although single-bonded carbon-oxygen groups (-OH and C-O-C) are more abundant on the GO basal plane and play an important role in Pt nanoparticle nucleation and distribution on graphene sheets, the double-bonded carbon-oxygen (C=O and COOH) groups are more abundant residual species post Pt nanoparticle growth and play a vital role in enhancing CO tolerance.",
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Sharma, S, Groves, MN, Fennell, J, Soin, N, Horswell, SL & Malardier-Jugroot, C 2014, 'Carboxyl group enhanced CO tolerant GO supported Pt catalysts: DFT and electrochemical analysis', Chemistry of Materials, vol. 26, no. 21, pp. 6142-6151. https://doi.org/10.1021/cm502447s

Carboxyl group enhanced CO tolerant GO supported Pt catalysts : DFT and electrochemical analysis. / Sharma, S.; Groves, M. N.; Fennell, J.; Soin, Navneet; Horswell, S. L.; Malardier-Jugroot, C.

In: Chemistry of Materials, Vol. 26, No. 21, 11.11.2014, p. 6142-6151.

Research output: Contribution to journalArticle

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T1 - Carboxyl group enhanced CO tolerant GO supported Pt catalysts

T2 - Chemistry of Materials

AU - Sharma, S.

AU - Groves, M. N.

AU - Fennell, J.

AU - Soin, Navneet

AU - Horswell, S. L.

AU - Malardier-Jugroot, C.

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N2 - The effect of residual oxygen species in as-prepared Pt nanoparticle on partially reduced graphene oxide (Pt/PRGO) and partially reduced carboxylated-GO (Pt/PR(GO-COOH)) supports was investigated using electrochemical CO stripping and density functional theory (DFT) analysis. Pt/PRGO and Pt/PR(GO-COOH) revealed a clear negative shift in CO-stripping onset potential compared to commercial Pt/carbon black. DFT analysis confirmed that the presence of a -COOH group provides the most resistance for CO adsorption. This CO-Pt binding energy is significantly lower than that observed in the presence of an OH group, which is the most abundant oxygen group in carbon supports. The Pt-CO dissociation energies (on a 42-atom graphene sheet) in the presence of various oxygen groups, in descending order, were OH > C=O ≈ C-O-C > COOH. Although single-bonded carbon-oxygen groups (-OH and C-O-C) are more abundant on the GO basal plane and play an important role in Pt nanoparticle nucleation and distribution on graphene sheets, the double-bonded carbon-oxygen (C=O and COOH) groups are more abundant residual species post Pt nanoparticle growth and play a vital role in enhancing CO tolerance.

AB - The effect of residual oxygen species in as-prepared Pt nanoparticle on partially reduced graphene oxide (Pt/PRGO) and partially reduced carboxylated-GO (Pt/PR(GO-COOH)) supports was investigated using electrochemical CO stripping and density functional theory (DFT) analysis. Pt/PRGO and Pt/PR(GO-COOH) revealed a clear negative shift in CO-stripping onset potential compared to commercial Pt/carbon black. DFT analysis confirmed that the presence of a -COOH group provides the most resistance for CO adsorption. This CO-Pt binding energy is significantly lower than that observed in the presence of an OH group, which is the most abundant oxygen group in carbon supports. The Pt-CO dissociation energies (on a 42-atom graphene sheet) in the presence of various oxygen groups, in descending order, were OH > C=O ≈ C-O-C > COOH. Although single-bonded carbon-oxygen groups (-OH and C-O-C) are more abundant on the GO basal plane and play an important role in Pt nanoparticle nucleation and distribution on graphene sheets, the double-bonded carbon-oxygen (C=O and COOH) groups are more abundant residual species post Pt nanoparticle growth and play a vital role in enhancing CO tolerance.

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