Quantitative Structure–Electrochemistry Relationship (QSER) Studies on Metal–Amino–Porphyrins for the Rational Design of CO2 Reduction Catalysts

The quantitative structure–electrochemistry relationship (QSER) method was applied to a series of transition-metal-coordinated porphyrins to relate their structural properties to their electrochemical CO2 reduction activity. Since the reactions mainly occur within the core of the metalloporphyrin ca...

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Bibliographic Details
Published in:Molecules (Basel, Switzerland) Switzerland), 2023-03, Vol.28 (7), p.3105
Main Authors: Chen, Furong, Wiriyarattanakul, Amphawan, Xie, Wanting, Shi, Liyi, Rungrotmongkol, Thanyada, Jia, Rongrong, Maitarad, Phornphimon
Format: Article
Language:English
Subjects:
Carbon
Carbon dioxide
catalyst design
Catalysts
Chemical reactions
CO2RR
Density functional theory
Dependent variables
DFT
Electrochemistry
Genetic algorithms
Hydrogen
Mathematical models
metalloporphyrin
Metals
Nitrogen atoms
Porphyrins
QSER
Reduction (metal working)
Statistical analysis
Transition metals
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Summary:The quantitative structure–electrochemistry relationship (QSER) method was applied to a series of transition-metal-coordinated porphyrins to relate their structural properties to their electrochemical CO2 reduction activity. Since the reactions mainly occur within the core of the metalloporphyrin catalysts, the cluster model was used to calculate their structural and electronic properties using density functional theory with the M06L exchange–correlation functional. Three dependent variables were employed in this work: the Gibbs free energies of H*, C*OOH, and O*CHO. QSER, with the genetic algorithm combined with multiple linear regression (GA–MLR), was used to manipulate the mathematical models of all three Gibbs free energies. The obtained statistical values resulted in a good predictive ability (R2 value) greater than 0.945. Based on our QSER models, both the electronic properties (charges of the metal and porphyrin) and the structural properties (bond lengths between the metal center and the nitrogen atoms of the porphyrin) play a significant role in the three Gibbs free energies. This finding was further applied to estimate the CO2 reduction activities of the metal–monoamino–porphyrins, which will prove beneficial in further experimental developments.
ISSN:1420-3049
1420-3049
DOI:10.3390/molecules28073105