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Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics

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The Solvent Effect on H₂ O₂ Generation at Room Temperature Ionic Liquid|Water Interface.

Justyna Kalisz¹, Wojciech Nogala¹, Wojciech Adamiak¹

¹Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224, Warsaw, Poland.

Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry

|April 28, 2021

Summary

Hydrogen peroxide (H₂ O₂) is produced at liquid interfaces using ionic liquids and decamethylferrocene. This study reveals cation expulsion during H₂ O₂ generation, indicating kinetic control.

Keywords:

ORR SECM decamethylferrocene ion transfer oxygen reduction

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Area of Science:

Electrochemistry
Materials Science
Chemical Engineering

Background:

Hydrogen peroxide (H₂ O₂) is a valuable chemical with diverse applications.
H₂ O₂ can be synthesized via the oxygen reduction reaction (ORR) in various solvent systems.
Room temperature ionic liquids (ILs) offer unique properties for electrochemical reactions.

Purpose of the Study:

To investigate H₂ O₂ generation at liquid-liquid interfaces.
To explore the role of hydrophobic ionic liquids in the oxygen reduction reaction.
To understand the mechanism of H₂ O₂ formation with decamethylferrocene (DMFc) as an electron donor.

Main Methods:

Utilized eleven hydrophobic ionic liquids (ILs) with acidic aqueous solutions.
Employed decamethylferrocene (DMFc) as the electron donor in a biphasic system.
Quantified H₂ O₂ using colorimetric detection and measured fluxes via scanning electrochemical microscopy (SECM).

Main Results:

Colorimetrically detectable amounts of H₂ O₂ were generated in systems with alkyl imidazolium hexafluorophosphate and tetraalkylammonium bis(trifluoromethylsulfonyl)imide ILs.
SECM measurements revealed H₂ O₂ fluxes near the liquid-liquid interface.
Observed cation expulsion into the aqueous phase during H₂ O₂ generation, unlike in molecular solvent systems.

Conclusions:

H₂ O₂ generation is feasible at hydrophobic IL-aqueous interfaces.
The reaction mechanism involves cation expulsion, suggesting a different pathway compared to molecular solvents.
Weak correlation between H₂ O₂ flux and redox potentials indicates the reaction is kinetically controlled.