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DOE OSTI · 2587330

A polysulfide/ferricyanide redox flow battery with extended cycling

Khabbaz, Mahla Sarfaraz [Purdue Univ., West Lafayette, IN (United States)]·Thakur, Anupma [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000178979229)·Maity, Dipak [Indiana Univ., Indianapolis, IN (United States)] (ORCID:0000000197920281)·Biabanialitappeh, Sepideh [Purdue Univ., West Lafayette, IN (United States)]·Mortha, Bhargava [Purdue Univ., West Lafayette, IN (United States)]·McKay, Joshua P. [Purdue Univ., West Lafayette, IN (United States)]·Parada, Gerardo [Purdue Univ., West Lafayette, IN (United States)]·Agarwal, Mangilal [Indiana Univ., Indianapolis, IN (United States)]·Zhang, Honghu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000317847825)·Zhang, Xin [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:000000032000858X)·Bazak, J. David [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000245993208)·Wei, Xiaoliang [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000276922357)
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Abstract

The inexpensive sulfur raw material is promising to enable cost-effective redox flow batteries for long duration energy storage. But the catastrophic through-membrane crossover of polysulfides remains a severe challenge resulting in irreversible performance degradation and short cycle life. In this work, we demonstrate that use of a permselective cation exchange membrane yields a two orders of magnitude enhancement in polysulfide retention compared to the benchmark Nafion membrane. Combined physico-chemical, spectroscopic, and microscopic analyses suggest more disordered sidechain structures, which lead to the more hydrophobic nature and smaller hydrophilic domains in the membrane. The microstructural features contribute to the effective mitigation of polysulfide crossover. As a result, the cycle life of polysulfide/ferricyanide flow cells is boosted over a substantially extended test time. This finding sheds light on the fundamental membrane factors that cause polysulfide permeation and can provide feasible directions in the development of permselective membranes for polysulfide flow batteries.

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36 MATERIALS SCIENCE

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Khabbaz, Mahla Sarfaraz [Purdue Univ., West Lafayette, IN (United States)], Thakur, Anupma [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000178979229), Maity, Dipak [Indiana Univ., Indianapolis, IN (United States)] (ORCID:0000000197920281), Biabanialitappeh, Sepideh [Purdue Univ., West Lafayette, IN (United States)], Mortha, Bhargava [Purdue Univ., West Lafayette, IN (United States)], McKay, Joshua P. [Purdue Univ., West Lafayette, IN (United States)], Parada, Gerardo [Purdue Univ., West Lafayette, IN (United States)], Agarwal, Mangilal [Indiana Univ., Indianapolis, IN (United States)], Zhang, Honghu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000317847825), Zhang, Xin [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:000000032000858X), Bazak, J. David [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000245993208), Wei, Xiaoliang [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000276922357). 2025-07-23. A polysulfide/ferricyanide redox flow battery with extended cycling. https://doi.org/10.1039/d5ta05404d

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DOE OSTI2026

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The transition to a flexible and reliable energy infrastructure, using electro-thermal energy generation technologies such as geothermal, concentrated solar power, and nuclear, usually demands simultaneous advancement of thermal energy storage (TES) to support on-demand electricity generation and industrial applications while mitigating the inherent intermittency of renewable energy sources and power outages from direct energy generation. Among TES technologies, thermochemical energy storage (TCES) based on calcium looping emerges as a compelling high-power energy storage candidate due to its high reaction enthalpy, compatibility with elevated operating temperatures, and abundance of low-cost materials. However, the long-term durability of calcium-based sorbents for TCES is hindered by surface sintering and particle aggregation, leading to performance degradation over repeated thermal cycles. This study explores a moisture hydration-based strategy to regenerate a degraded calcium sorbent and mitigate performance degradation for long duration TCES. The addition of moisture transforms calcium oxide into calcium hydroxide and produces intercalation water layers, associated with a regenerated surface area and reduced calcium oxide crystallite size. Both these effects are beneficial in restoring the sorbents' reactivity for carbonization. Additionally, an optimized hydration-assisted reactivation protocol balances the recovered energy storage capacity with heating penalty required for moisture removal from hydrated samples, resulting in an enhanced energy storage capacity up to 176% compared to benchmark sorbents that undergo cycling without reactivation after 60 cycles. In conclusion, these results highlight the potential of hydration-assisted reactivation to enhance the long-term performance of TCES, providing an effective pathway to advancing electro-thermal storage technologies.

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