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Computational mechanistic investigation of the Fe + CO2→ FeO + CO reaction.
Dias Vicentini, Eduardo; de Lima Batista, Ana P; Sampaio de Oliveira-Filho, Antonio G.
Afiliación
  • Dias Vicentini E; Departamento de Química, Laboratório Computacional de Espectroscopia e Cinética, Faculdade de Filosofia, Ciências e Letras de Ribeirão Preto, Universidade de São Paulo, 14040-901, Ribeirão Preto-SP, Brazil. antoniogsof@ffcrp.usp.br.
Phys Chem Chem Phys ; 22(29): 16943-16948, 2020 Aug 07.
Article en En | MEDLINE | ID: mdl-32672262
We report a computational study of the mechanism and determination of the rate constants of the Fe + CO2→ FeO + CO reaction, in the 1000-3000 K temperature range, at the CCSD(T)/CBS//B3LYP/def2-TZVP level of theory. The overall rate constant was obtained by a Kinetic Monte Carlo simulation. The calculated rate constant, at 2000 K, is 9.72 × 10-13 cm3 molecule-1 s-1, in agreement with experimental measurements: 2.97 × 10-13 cm3 molecule-1 s-1 [A. Giesen et al., Phys. Chem. Chem. Phys., 2002, 4, 3665] and 1.13 × 10-13 cm3 molecule-1 s-1 [V. N. Smirnov, Kinet. Catal., 2008, 49, 607]. Our study shows that this reaction follows a complex mechanism, with multiple reaction paths contributing to the overall rate, and that CCSD(T) accurately describes this transition metal reaction.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Phys Chem Chem Phys Asunto de la revista: BIOFISICA / QUIMICA Año: 2020 Tipo del documento: Article País de afiliación: Brasil Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Phys Chem Chem Phys Asunto de la revista: BIOFISICA / QUIMICA Año: 2020 Tipo del documento: Article País de afiliación: Brasil Pais de publicación: Reino Unido