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

05 March 2020, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

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.

Keywords

hydrogen evolution reaction
hydrogen bond
cation effect
organic electrolyte
water splitting
water reduction
solvation effect

Supplementary materials

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Tuning the water reduction through controlled nanoconfinement within an organic liquid matrix SI
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