Influence of sp3-sp2 carbon nanodomains on metal/support interaction, catalyst durability, and catalytic activity for the oxygen reduction reaction

Carlos A. Campos-Roldán, Guadalupe Ramos-Sánchez, Rosa G. Gonzalez-Huerta, Jorge R. Vargas García, Perla B. Balbuena, Nicolas Alonso-Vante

Research output: Contribution to journalArticle

29 Citations (Scopus)

Abstract

© 2016 American Chemical Society. In this work, platinum nanoparticles were impregnated by two different techniques, namely the carbonyl chemical route and photodeposition, onto systematically surface-modified multiwalled carbon nanotubes. The different interactions between platinum nanoparticles with sp2-sp3 carbon nanodomains were investigated. The oxidation of an adsorbed monolayer of carbon monoxide, used to probe electronic catalytic modification, suggests a selective nucleation of platinum nanoparticles onto sp2 carbon nanodomains when photodeposition synthesis is carried out. XPS attests the catalytic center electronic modification obtained by photodeposition. DFT calculations were used to determine the interaction energy of a Pt cluster with sp2 and sp3 carbon surfaces as well as with oxidized ones. The interaction energy and electronic structure of the platinum cluster presents dramatic changes as a function of the support surface chemistry, which also modifies its catalytic properties evaluated by the interaction with CO. The interaction energy was calculated to be 8-fold higher on sp3 and oxidized surfaces in comparison to sp2 domains. Accelerated Stability Test (AST) was applied only on the electronic-modified materials to evaluate the active phase degradation and their activity toward oxygen reduction reaction (ORR). The stability of photodeposited materials is correlated with the surface chemical nature of supports indicating that platinum nanoparticles supported onto multiwalled carbon nanotubes with the highest sp2 character show the higher stability and activity toward ORR.
Original languageAmerican English
Pages (from-to)23260-23269
Number of pages20933
JournalACS Applied Materials and Interfaces
DOIs
StatePublished - 7 Sep 2016

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Platinum
Catalyst supports
Catalyst activity
Durability
Carbon
Metals
Oxygen
Catalysts
Nanoparticles
Multiwalled carbon nanotubes (MWCN)
Carbon Monoxide
Surface chemistry
Discrete Fourier transforms
Carbon monoxide
Electronic structure
Monolayers
Nucleation
Thermodynamic properties
X ray photoelectron spectroscopy
Degradation

Cite this

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title = "Influence of sp3-sp2 carbon nanodomains on metal/support interaction, catalyst durability, and catalytic activity for the oxygen reduction reaction",
abstract = "{\circledC} 2016 American Chemical Society. In this work, platinum nanoparticles were impregnated by two different techniques, namely the carbonyl chemical route and photodeposition, onto systematically surface-modified multiwalled carbon nanotubes. The different interactions between platinum nanoparticles with sp2-sp3 carbon nanodomains were investigated. The oxidation of an adsorbed monolayer of carbon monoxide, used to probe electronic catalytic modification, suggests a selective nucleation of platinum nanoparticles onto sp2 carbon nanodomains when photodeposition synthesis is carried out. XPS attests the catalytic center electronic modification obtained by photodeposition. DFT calculations were used to determine the interaction energy of a Pt cluster with sp2 and sp3 carbon surfaces as well as with oxidized ones. The interaction energy and electronic structure of the platinum cluster presents dramatic changes as a function of the support surface chemistry, which also modifies its catalytic properties evaluated by the interaction with CO. The interaction energy was calculated to be 8-fold higher on sp3 and oxidized surfaces in comparison to sp2 domains. Accelerated Stability Test (AST) was applied only on the electronic-modified materials to evaluate the active phase degradation and their activity toward oxygen reduction reaction (ORR). The stability of photodeposited materials is correlated with the surface chemical nature of supports indicating that platinum nanoparticles supported onto multiwalled carbon nanotubes with the highest sp2 character show the higher stability and activity toward ORR.",
author = "Campos-Rold{\'a}n, {Carlos A.} and Guadalupe Ramos-S{\'a}nchez and Gonzalez-Huerta, {Rosa G.} and {Vargas Garc{\'i}a}, {Jorge R.} and Balbuena, {Perla B.} and Nicolas Alonso-Vante",
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Influence of sp3-sp2 carbon nanodomains on metal/support interaction, catalyst durability, and catalytic activity for the oxygen reduction reaction. / Campos-Roldán, Carlos A.; Ramos-Sánchez, Guadalupe; Gonzalez-Huerta, Rosa G.; Vargas García, Jorge R.; Balbuena, Perla B.; Alonso-Vante, Nicolas.

In: ACS Applied Materials and Interfaces, 07.09.2016, p. 23260-23269.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Influence of sp3-sp2 carbon nanodomains on metal/support interaction, catalyst durability, and catalytic activity for the oxygen reduction reaction

AU - Campos-Roldán, Carlos A.

AU - Ramos-Sánchez, Guadalupe

AU - Gonzalez-Huerta, Rosa G.

AU - Vargas García, Jorge R.

AU - Balbuena, Perla B.

AU - Alonso-Vante, Nicolas

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N2 - © 2016 American Chemical Society. In this work, platinum nanoparticles were impregnated by two different techniques, namely the carbonyl chemical route and photodeposition, onto systematically surface-modified multiwalled carbon nanotubes. The different interactions between platinum nanoparticles with sp2-sp3 carbon nanodomains were investigated. The oxidation of an adsorbed monolayer of carbon monoxide, used to probe electronic catalytic modification, suggests a selective nucleation of platinum nanoparticles onto sp2 carbon nanodomains when photodeposition synthesis is carried out. XPS attests the catalytic center electronic modification obtained by photodeposition. DFT calculations were used to determine the interaction energy of a Pt cluster with sp2 and sp3 carbon surfaces as well as with oxidized ones. The interaction energy and electronic structure of the platinum cluster presents dramatic changes as a function of the support surface chemistry, which also modifies its catalytic properties evaluated by the interaction with CO. The interaction energy was calculated to be 8-fold higher on sp3 and oxidized surfaces in comparison to sp2 domains. Accelerated Stability Test (AST) was applied only on the electronic-modified materials to evaluate the active phase degradation and their activity toward oxygen reduction reaction (ORR). The stability of photodeposited materials is correlated with the surface chemical nature of supports indicating that platinum nanoparticles supported onto multiwalled carbon nanotubes with the highest sp2 character show the higher stability and activity toward ORR.

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