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Tuning the Water Reduction Through Controlled Nanoconfinement Within an Organic Liquid Matrix

preprint
revised on 29.05.2020 and posted on 01.06.2020 by Nicolas Dubouis, Alessandra Serva, Roxanne Berthin, Guillaume Jeanmairet, Benjamin Porcheron, Elodie Salager, Mathieu Salanne, Alexis Grimaud

The growing hydrogen-economy requires accelerating the hydrogen evolution reaction. The water dissociation step (Volmer step) has been proposed as a main kinetic limitation, but the mechanisms at play in the electrochemical double-layer are poorly understood. This is due to the ambivalent role of water: it acts both as a reactant and as a solvent. Here we propose to confine water inside an organic liquid matrix in order to isolate the sole role of water as a reactant. We observe the formation of aqueous-rich nanodomains, which size can be tuned by changing the supporting electrolyte, and found that the reactivity of the system significantly varies with its nanostructure. Depending on the conditions, it is dominated by either the strength of short-range cation-water interactions or the formation of long chains of water molecules. This understanding paves the way toward the development of more efficient and selective electrocatalysts for the water, CO2, O2 or N2 reduction.

Funding

ANR-10LABX-76-01

European Research Council 771294

History

Email Address of Submitting Author

alexis.grimaud@college-de-france.fr

Institution

Chimie du Solide et de l’Energie, Collège de France

Country

France

ORCID For Submitting Author

0000-0002-9966-205X

Declaration of Conflict of Interest

The authors declare no competing interests

Version Notes

Submitted version Molecular dynamics input, intial and final configurations

Exports