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
N1 - Publisher Copyright:
© 2016 American Chemical Society.
PY - 2016/9/7
Y1 - 2016/9/7
N2 - 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.
AB - 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.
KW - DFT
KW - ORR
KW - durability
KW - electrocatalyst
KW - sp-sp domains
UR - http://www.scopus.com/inward/record.url?scp=84986598311&partnerID=8YFLogxK
U2 - 10.1021/acsami.6b06886
DO - 10.1021/acsami.6b06886
M3 - Artículo
SN - 1944-8244
VL - 8
SP - 23260
EP - 23269
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 35
ER -