Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.181
Publication date: 16th December 2024
The concept of concentrated aqueous solutions, referred as water-in-salt electrolytes (WISEs),1 brought back recently the interest in aqueous batteries. These electrolytes can be described as few water molecules surrounded by cations and anions. The limited amount of free water molecules, the particular interfaces created,2 as well as the change of the solvation structure strongly modify the solutions behavior. Consequently, the electrochemical stability window is largely extended up to more than 3 V. Multiple strategies have been implemented to extend further the stability window by occupying the water molecules, with the addition of a co-salt (bi-salt electrolyte)3 or the presence of a molecular crowding agent such as a polymer.4 These strategies strongly impact the organization of the water molecules in solution. Similarly, the kosmotropic or chaotropic character of the salt anion5 affects the water network, with the chaotropic anions being more efficient in disturbing the water molecules. Yet, the importance of such strategies on the long-term reactivity of aqueous batteries,6 particularly on the challenging limitation of the hydrogen evolution reaction (HER) at the cathodic side, has yet to be fully demonstrated.
In this context, we performed a screening of the gas production in full magnesium cells as a function of the electrolyte’s nature: imide,7 acetate or perchlorate-based electrolytes, bi-salt electrolytes and polymer-based electrolytes. In particular, we focused on H2 production, used as a universal criterion to assess the relevance of the solutions considered.
At low molalities, we found that the production of H2 follows the kosmo/chaotropic classification of the anions. However, at the highest molalities (or lowest water-to-anion ratios), a similar trend for the production of H2 is observed, whatever the electrolyte considered. While the nature of the anion has a major influence on the solution’s organization, ultimately the H2 production and reactivity seems only guided by the quantity of water in solution.
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