Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.172
Publication date: 22nd December 2022
The omnipresent Li-ion batteries are reaching their energy density limitations. At the same time, energy storage demands are drastically increasing, motivating researchers to pursue new battery systems. Due to the bivalent nature of ions, low redox potentials, high gravimetric capacities, and natural abundance, Mg and Ca metal anode batteries are considered as promising post-Li energy storage systems. One of the main challenges of both systems is the development of electrolytes.
Fluorinated alkoxyborate-based electrolytes were introduced into Mg and Ca batteries a few years ago and presented significant progress over the previous generations of electrolytes in terms of overpotentials, stability, and Cl-free character.1 Specifically, Mg[B(hfip)4]2 and Ca[B(hfip)4]2 (hfip = 1,1,1,3,3,3–hexafluoroisopropoxy) served as model compounds to show that weakly coordinated anion with a high degree of fluorination enables large charge delocalization, decreases the anion–cation interaction, and consequently reduces the ion-pair formation.2 Additional improvement for Mg batteries has been reached with the introduction of Mg fluorinated alkoxyaluminate electrolytes. Among those, Mg[Al(hfip)4]2 with Coulombic efficiency over 99.5% and overpotentials below 60 mV is considered a state-of-the-art Mg electrolyte.3
In our research, we explore the field of fluorinated alkoxy electrolytes by synthesizing Mg alkoxyborates with exchanged hfip ligand for various alcohols with different sterical properties, number of binding groups, and degree of fluorination. Additionally, a synthesis of a novel Ca[Al(hfip)4]2 salt is developed. All electrolytes are studied by extensive physicochemical and electrochemical characterization. Our study shows that changing the anion structure allows the development of electrolytes offering improved electrochemical performance compared to the model [B(hfip)4]2– – based electrolytes and exposes the most promising candidates for further studies for practical Mg and Ca rechargeable batteries.
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