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Energetics of CO2- in Aqueous Solution.

Ashley S McNeill1, David A Dixon1

  • 1Department of Chemistry and Biochemistry , The University of Alabama , Shelby Hall , Box 870336, Tuscaloosa , Alabama 35487-0336 , United States.

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Anionic carbon dioxide (CO2-) clusters are more stable than neutral ones, especially in water. This study predicts a high electron affinity for aqueous CO2-, indicating significant solvent reorganization upon electron transfer.

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Area of Science:

  • Computational Chemistry
  • Physical Chemistry
  • Quantum Chemistry

Background:

  • Understanding the behavior of anionic species in solution is crucial for various chemical processes.
  • Carbon dioxide (CO2) is a ubiquitous molecule, and its anionic form (CO2-) plays a role in electrochemical reactions and atmospheric chemistry.
  • The influence of solvation, particularly by water molecules, on the electronic properties and stability of anions is a key area of research.

Purpose of the Study:

  • To investigate the energetic stability of neutral and anionic CO2 clusters with explicit water molecules in both gas and aqueous phases.
  • To determine the adiabatic electron affinity (EA) of CO2 in aqueous solution and its dependence on the number of hydrating water molecules.
  • To explore the structural and electronic changes of the CO2- anion upon electron attachment/detachment in a solvated environment.

Main Methods:

  • High-level ab initio calculations using the coupled cluster (CCSD(T)) method.
  • Inclusion of solvent effects via a self-consistent reaction field (SCRF) model.
  • Calculation of various energy metrics including gas-phase enthalpies (ΔHgas), aqueous free energies (ΔGaq), adiabatic electron affinities (EA), and vertical attachment/detachment energies.

Main Results:

  • Anionic CO2 clusters are energetically more favorable than neutral clusters, with greater stabilization in aqueous solution.
  • The adiabatic electron affinity of aqueous CO2- is predicted to be 2.35 ± 0.08 eV, converging with as few as three water molecules.
  • The CO2- anion adopts a bent structure (135°) in solution, requiring significant energy for bending and indicating substantial solvent reorganization during electron transfer.

Conclusions:

  • The enhanced stability of anionic CO2 in aqueous solution is attributed to strong hydrogen bonding interactions with water molecules.
  • The calculated EA of aqueous CO2- is significantly higher than the solvation free energy of the electron, highlighting the importance of specific solute-solvent interactions.
  • Dimerization of CO2- to form aqueous C2O4(2-) is predicted to occur, suggesting potential reaction pathways in aqueous environments.