Catalytic activity toward oxygen reduction of transition metal porphyrins covalently linked to single-walled carbon nanotubes: A density functional study

Resultado de la investigación: Article

15 Citas (Scopus)

Resumen

The interaction of molecular oxygen with the metal center of transition metal porphyrins (MP, with M = Mn, Fe, Co, and Ni) covalently linked to single-walled carbon nanotubes (CNTs) are addressed by density functional theory calculations. Two geometries for the CNT sidewall functionalization with porphyrin radicals are proposed, considering sp2 and sp3 chemical bonds. By computing the stability and electronic properties of the CNT-MP complexes, and the interaction of the O2 molecule with the metal center, we investigate their catalytic activity toward the oxygen reduction reaction (ORR). According to our results, CNT-MnP, CNT-CoP, and CNT-FeP linked by sp2 covalent bonds are highly stable, preserving the CNT metallic character. We also find a significant O-O bond weakening after the oxygen adsorption on the porphyrin metal center, showing favorable conditions toward ORR. These results support experimental evidences of ORR activity in CNT-based transition metal-N 4 centers.

Idioma originalEnglish
Número de artículo155405
PublicaciónPhysical Review B - Condensed Matter and Materials Physics
Volumen84
N.º15
DOI
EstadoPublished - 7 oct 2011

Huella dactilar

Carbon Nanotubes
Porphyrins
Single-walled carbon nanotubes (SWCN)
porphyrins
Transition metals
catalytic activity
Catalyst activity
Carbon nanotubes
transition metals
carbon nanotubes
Oxygen
oxygen
Metals
metals
Covalent bonds
Molecular oxygen
Chemical bonds
covalent bonds
Electronic properties
chemical bonds

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Electronic, Optical and Magnetic Materials

Citar esto

@article{b0f65b47877d406fa294f1afefc41f4d,
title = "Catalytic activity toward oxygen reduction of transition metal porphyrins covalently linked to single-walled carbon nanotubes: A density functional study",
abstract = "The interaction of molecular oxygen with the metal center of transition metal porphyrins (MP, with M = Mn, Fe, Co, and Ni) covalently linked to single-walled carbon nanotubes (CNTs) are addressed by density functional theory calculations. Two geometries for the CNT sidewall functionalization with porphyrin radicals are proposed, considering sp2 and sp3 chemical bonds. By computing the stability and electronic properties of the CNT-MP complexes, and the interaction of the O2 molecule with the metal center, we investigate their catalytic activity toward the oxygen reduction reaction (ORR). According to our results, CNT-MnP, CNT-CoP, and CNT-FeP linked by sp2 covalent bonds are highly stable, preserving the CNT metallic character. We also find a significant O-O bond weakening after the oxygen adsorption on the porphyrin metal center, showing favorable conditions toward ORR. These results support experimental evidences of ORR activity in CNT-based transition metal-N 4 centers.",
author = "Walter Orellana",
year = "2011",
month = "10",
day = "7",
doi = "10.1103/PhysRevB.84.155405",
language = "English",
volume = "84",
journal = "Physical Review B-Condensed Matter",
issn = "1098-0121",
publisher = "American Physical Society",
number = "15",

}

TY - JOUR

T1 - Catalytic activity toward oxygen reduction of transition metal porphyrins covalently linked to single-walled carbon nanotubes

T2 - A density functional study

AU - Orellana, Walter

PY - 2011/10/7

Y1 - 2011/10/7

N2 - The interaction of molecular oxygen with the metal center of transition metal porphyrins (MP, with M = Mn, Fe, Co, and Ni) covalently linked to single-walled carbon nanotubes (CNTs) are addressed by density functional theory calculations. Two geometries for the CNT sidewall functionalization with porphyrin radicals are proposed, considering sp2 and sp3 chemical bonds. By computing the stability and electronic properties of the CNT-MP complexes, and the interaction of the O2 molecule with the metal center, we investigate their catalytic activity toward the oxygen reduction reaction (ORR). According to our results, CNT-MnP, CNT-CoP, and CNT-FeP linked by sp2 covalent bonds are highly stable, preserving the CNT metallic character. We also find a significant O-O bond weakening after the oxygen adsorption on the porphyrin metal center, showing favorable conditions toward ORR. These results support experimental evidences of ORR activity in CNT-based transition metal-N 4 centers.

AB - The interaction of molecular oxygen with the metal center of transition metal porphyrins (MP, with M = Mn, Fe, Co, and Ni) covalently linked to single-walled carbon nanotubes (CNTs) are addressed by density functional theory calculations. Two geometries for the CNT sidewall functionalization with porphyrin radicals are proposed, considering sp2 and sp3 chemical bonds. By computing the stability and electronic properties of the CNT-MP complexes, and the interaction of the O2 molecule with the metal center, we investigate their catalytic activity toward the oxygen reduction reaction (ORR). According to our results, CNT-MnP, CNT-CoP, and CNT-FeP linked by sp2 covalent bonds are highly stable, preserving the CNT metallic character. We also find a significant O-O bond weakening after the oxygen adsorption on the porphyrin metal center, showing favorable conditions toward ORR. These results support experimental evidences of ORR activity in CNT-based transition metal-N 4 centers.

UR - http://www.scopus.com/inward/record.url?scp=80455178829&partnerID=8YFLogxK

U2 - 10.1103/PhysRevB.84.155405

DO - 10.1103/PhysRevB.84.155405

M3 - Article

AN - SCOPUS:80455178829

VL - 84

JO - Physical Review B-Condensed Matter

JF - Physical Review B-Condensed Matter

SN - 1098-0121

IS - 15

M1 - 155405

ER -