Issue 48, 2021

Computational and experimental investigation of the effect of cation structure on the solubility of anionic flow battery active-materials

Abstract

Recent advances in clean, sustainable energy sources such as wind and solar have enabled significant cost improvements, yet their inherent intermittency remains a considerable challenge for year-round reliability demanding the need for grid-scale energy storage. Nonaqueous redox flow batteries (NRFBs) have the potential to address this need, with attractive attributes such as flexibility to accommodate long- and short-duration storage, separately scalable energy and power ratings, and improved safety profile over integrated systems such as lithium-ion batteries. Currently, the low-solubility of NRFB electrolytes fundamentally limits their energy density. However, synthetically exploring the large chemical and parameter space of NRFB active materials is not only costly but also intractable. Here, we report a computational framework, coupled with experimental validation, designed to predict the solubility trends of electrolytes, incorporating both the lattice and solvation free energies. We reveal that lattice free energy, which has previously been neglected, has a significant role in tuning electrolyte solubility, and that solvation free energies alone is insufficient. The desymmetrization of the alkylammonium cation leading to short-chain, asymmetric cations demonstrated a modest increase in solubility, which can be further explored for NRFB electrolyte development and optimization. The resulting synergistic computational–experimental approach provides a cost-effective strategy in the development of high-solubility active materials for high energy density NRFB systems.

Graphical abstract: Computational and experimental investigation of the effect of cation structure on the solubility of anionic flow battery active-materials

Supplementary files

Article information

Article type
Edge Article
Submitted
09 9 2021
Accepted
24 11 2021
First published
26 11 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2021,12, 15892-15907

Computational and experimental investigation of the effect of cation structure on the solubility of anionic flow battery active-materials

B. R. B. Visayas, S. K. Pahari, T. C. Gokoglan, J. A. Golen, E. Agar, P. J. Cappillino and M. L. Mayes, Chem. Sci., 2021, 12, 15892 DOI: 10.1039/D1SC04990A

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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