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Density functional theory and 3D-RISM-KH molecular theory of solvation studies of CO2 reduction on Cu-, Cu2O-, Fe-, and Fe3O4-based nanocatalysts

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Abstract

Using OpenMX quantum chemistry software for self-consistent field calculations of electronic structure with geometry optimization and 3D-RISM-KH molecular theory of solvation for 3D site distribution functions and solvation free energy, we modeled the reduction of CO2+H2 in ambient aqueous electrolyte solution of 1.0-M KH2PO4 into (i) formic acid HCOOH and (ii) CO H2O on the surfaces of Cu-, Fe-, Cu2O-, and Fe3O4-based nanocatalysts. It is applicable to its further reduction to hydrocarbons. The optimized geometries and free energies were obtained for the pathways of adsorption of the reactants from the solution, successive reduction on the surfaces of the nanocatalysts, and then release back to the solution bulk.

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Acknowledgments

Generous computing time provided by Compute Canada/Calcul Canada (www.computecanada.ca) is acknowledged.

Funding

This work was financially supported by the National Research Council of Canada, Research Grant A1-015524-01 0002.

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Authors and Affiliations

  1. Nanotechnology Research Centre, National Research Council of Canada, 11421 Saskatchewan Drive, Edmonton, Alberta, T6G 2M9, Canada

    Andriy Kovalenko

  2. Department of Mechanical Engineering, University of Alberta, 10-203 Donadeo Innovation Centre for Engineering, 9211-116 Str., Edmonton, Alberta, T6G 1H9, Canada

    Andriy Kovalenko

  3. Institute for Fuel Cell Innovation, Energy, Mining & Environment, National Research Council of Canada, 4250 Wesbrook Mall, Vancouver, British Columbia, V6T 1W5, Canada

    Vladimir Neburchilov

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  1. Andriy Kovalenko
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  2. Vladimir Neburchilov
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Correspondence to Andriy Kovalenko.

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Kovalenko, A., Neburchilov, V. Density functional theory and 3D-RISM-KH molecular theory of solvation studies of CO2 reduction on Cu-, Cu2O-, Fe-, and Fe3O4-based nanocatalysts. J Mol Model 26, 267 (2020). https://doi.org/10.1007/s00894-020-04529-8

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  • DOI: https://doi.org/10.1007/s00894-020-04529-8

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