am6b06886_si_001.pdf (377.4 kB)
Influence of sp3–sp2 Carbon Nanodomains on Metal/Support Interaction, Catalyst Durability, and Catalytic Activity for the Oxygen Reduction Reaction
journal contribution
posted on 2016-08-05, 00:00 authored by Carlos A. Campos-Roldán, Guadalupe Ramos-Sánchez, Rosa G. Gonzalez-Huerta, Jorge R. Vargas García, Perla B. Balbuena, Nicolas Alonso-VanteIn
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.
History
Usage metrics
Categories
Keywords
sp 2 domainssp 3 carbon surfacesXPSOxygen Reduction ReactionORRcarbonyl chemical routesupport surface chemistrysurface-modified multiwalled carbon nanotubesmultiwalled carbon nanotubesoxygen reduction reactionsp 2 carbon nanodomainsASTCODFTplatinum nanoparticlessp 2 character showinteraction energysurface chemical nature
Licence
Exports
RefWorks
BibTeX
Ref. manager
Endnote
DataCite
NLM
DC