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Article

The Role of Redox Potential and Molecular Structure of Co(II)-Polypyridine Complexes on the Molecular Catalysis of CO2 Reduction

by
Juan Pablo F. Rebolledo-Chávez
1,
Gionnany Teodoro Toral
1,
Vanesa Ramírez-Delgado
1,
Yolanda Reyes-Vidal
1,
Martha L. Jiménez-González
1,
Marisela Cruz-Ramírez
2,
Angel Mendoza
3 and
Luis Ortiz-Frade
1,*
1
Centro de Investigación y Desarrollo Tecnológico en Electroquímica S.C. Parque Tecnológico Querétaro, Departamento de Electroquímica, 76703 Santiago de Querétaro, Mexico
2
División de Química y Energías Renovables, Universidad Tecnológica de San Juan del Río, 76800 San Juan del Río, Mexico
3
Centro de Química, Instituto de Ciencias, Benemérita Universidad Autónoma de Puebla, Ciudad Universitaria, Col. San Manuel, 72570 Puebla, Mexico
*
Author to whom correspondence should be addressed.
Catalysts 2021, 11(8), 948; https://doi.org/10.3390/catal11080948
Submission received: 30 June 2021 / Revised: 27 July 2021 / Accepted: 4 August 2021 / Published: 8 August 2021
(This article belongs to the Special Issue Advances in Applied Electrocatalysis)
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Abstract

In this work, we report the electrochemical response of a family of Co(II) complexes, [CoII(L)3]2+ and [CoII(L’)2]2+ (L = 2,2’-bipyridine, 1,10-phenanthroline, 3,4,7,8-tetramethyl-1,10-phenanthroline, 5,6-dimethyl-1,10-phenanthroline, and 4,7-diphenyl-1,10-phenanthroline; L’ = terpyridine and 4-chloro-terpyridine), in the presence and absence of CO2 in order to understand the role of the redox potential and molecular structure on the molecular catalysis of CO2 reduction. The tris chelate complexes exhibited three electron transfer processes [CoII(L)3]2+ ⇄ [CoIII(L)3]3+ + 1e−, [CoΙΙ(L)3]2++1e− ⇄ [CoΙ(L)3]+, and [CoΙ(L)3]+ + 2e- ⇄ [CoΙ(L)(L−)2]−. In the case of complexes with 1,10-phen and 2,2-bipy, the third redox process showed a coupled chemical reaction [CoΙ(L)(L−)2]− → [CoΙ(L−)2]− + L. For bis chelate complexes, three electron transfer processes associated with the redox couples [CoΙΙ(L)2]/[CoIII(L)2]3+, [CoΙΙ(L)2]2+/[CoΙ(L)2]+, and [CoΙ(L)2]+/[CoΙ(L)(L−)] were registered, including a coupled chemical reaction only for the complex containing the ligand 4-chloro-terpyridine. Foot to the wave analysis (FOWA) obtained from cyclic voltammetry experiments allowed us to calculate the catalytic rate constant (k) for the molecular catalysis of CO2 reduction. The complex [Co(3,4,7,8-tm-1,10-phen)3]2+ presented a high k value; moreover, the complex [Co(4-Cl-terpy)3]2+ did not show catalytic activity, indicating that the more negative redox potential and the absence of the coupled chemical reaction increased the molecular catalysis. Density functional theory (DFT) calculations for compounds and CO2 were obtained to rationalize the effect of electronic structure on the catalytic rate constant (k) of CO2 reduction.
Keywords: molecular catalysis; CO2 reduction; Co(II)-polypyridine complexes; DFT calculations molecular catalysis; CO2 reduction; Co(II)-polypyridine complexes; DFT calculations
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MDPI and ACS Style

Rebolledo-Chávez, J.P.F.; Toral, G.T.; Ramírez-Delgado, V.; Reyes-Vidal, Y.; Jiménez-González, M.L.; Cruz-Ramírez, M.; Mendoza, A.; Ortiz-Frade, L. The Role of Redox Potential and Molecular Structure of Co(II)-Polypyridine Complexes on the Molecular Catalysis of CO2 Reduction. Catalysts 2021, 11, 948. https://doi.org/10.3390/catal11080948

AMA Style

Rebolledo-Chávez JPF, Toral GT, Ramírez-Delgado V, Reyes-Vidal Y, Jiménez-González ML, Cruz-Ramírez M, Mendoza A, Ortiz-Frade L. The Role of Redox Potential and Molecular Structure of Co(II)-Polypyridine Complexes on the Molecular Catalysis of CO2 Reduction. Catalysts. 2021; 11(8):948. https://doi.org/10.3390/catal11080948

Chicago/Turabian Style

Rebolledo-Chávez, Juan Pablo F., Gionnany Teodoro Toral, Vanesa Ramírez-Delgado, Yolanda Reyes-Vidal, Martha L. Jiménez-González, Marisela Cruz-Ramírez, Angel Mendoza, and Luis Ortiz-Frade. 2021. "The Role of Redox Potential and Molecular Structure of Co(II)-Polypyridine Complexes on the Molecular Catalysis of CO2 Reduction" Catalysts 11, no. 8: 948. https://doi.org/10.3390/catal11080948

APA Style

Rebolledo-Chávez, J. P. F., Toral, G. T., Ramírez-Delgado, V., Reyes-Vidal, Y., Jiménez-González, M. L., Cruz-Ramírez, M., Mendoza, A., & Ortiz-Frade, L. (2021). The Role of Redox Potential and Molecular Structure of Co(II)-Polypyridine Complexes on the Molecular Catalysis of CO2 Reduction. Catalysts, 11(8), 948. https://doi.org/10.3390/catal11080948

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