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DOE OSTI · 2570579

Designing Moderately‐Solvating Electrolytes for High‐Performance Lithium–Sulfur Batteries

Kautz, David J. [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000230092933)·Cao, Xia [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000316104341)·Gao, Peiyuan [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000229066551)·Feng, Shuo [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)]·Zhao, Qian [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)] (ORCID:0000000344893691)·Parab, Saurabh [Univ. of California, San Diego, CA (United States)] (ORCID:0000000307606155)·Xu, Yaobin [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000299453514)·Quinn, Joseph P. [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)]·Rahman, Muhammad Mominur [Brookhaven National Laboratory (BNL), Upton, NY (United States)]·Tan, Sha [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:000000018277893X)·Zhang, Xin [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:000000032000858X)·Ketabi, Sanaz [General Motors R&D, Warren, MI (United States)] (ORCID:0009000258534948)·Nazir, Aqsa [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000330752476)·Wang, Junxia [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)]·Dai, Fang [General Motors R&D, Warren, MI (United States)] (ORCID:0000000292295576)·Wang, Shen [Univ. of California, San Diego, CA (United States)] (ORCID:0000000338264397)·Lu, Dongping [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000195978500)·Hu, Enyuan [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000218814534)·Meng, Y. Shirley [Univ. of California, San Diego, CA (United States)] (ORCID:0000000189368845)·Wang, Chongmin [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)] (ORCID:0000000333270958)·Liu, Jun [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)] (ORCID:0000000186637771)·Zhang, Ji‐Guang [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000173434609)·Xu, Wu [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000226858684)
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Abstract

New electrolytes are critical for high‐energy lithium (Li)–sulfur (S) batteries (LSBs) to ensure their stability against Li metal anode and polysulfides (PSs) shuttling which hinder the large‐scale application of LSBs. In this study, the design principle of moderately solvating electrolytes (MSEs) for LSBs is demonstrated by using a multiple‐solvent system comprising of a highly solvating solvent, a weakly solvating solvent, and a non‐solvating solvent to create a well‐balanced electrolyte system. This resulting electrolyte significantly improves the cycle life of LSBs, achieving 300 cycles, which is twice as long as that of similar cells with the conventional electrolyte and it also ensures stable calendar life for at least seven months. The optimal MSE forms robust passivation layers enhancing the structural integrity of both S and Li metal electrodes after cycling. These virtues effectively hinder parasitic side reactions and self‐discharge behavior of LSBs. This electrolyte design principle is versatile and can be applied to other battery chemistries, providing a potential path toward the development of a more efficient and stable battery system. By addressing key challenges such as the instability of electrodes and shuttling of polysulfides, this electrolyte approach offers promising solutions for advancing LSB technology.

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25 ENERGY STORAGEcycle and calendar lifelithium-sulfur batterymoderately solvating electrolytepolysulfideself-discharge

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Kautz, David J. [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000230092933), Cao, Xia [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000316104341), Gao, Peiyuan [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000229066551), Feng, Shuo [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)], Zhao, Qian [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)] (ORCID:0000000344893691), Parab, Saurabh [Univ. of California, San Diego, CA (United States)] (ORCID:0000000307606155), Xu, Yaobin [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000299453514), Quinn, Joseph P. [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)], Rahman, Muhammad Mominur [Brookhaven National Laboratory (BNL), Upton, NY (United States)], Tan, Sha [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:000000018277893X), Zhang, Xin [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:000000032000858X), Ketabi, Sanaz [General Motors R&D, Warren, MI (United States)] (ORCID:0009000258534948), Nazir, Aqsa [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000330752476), Wang, Junxia [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)], Dai, Fang [General Motors R&D, Warren, MI (United States)] (ORCID:0000000292295576), Wang, Shen [Univ. of California, San Diego, CA (United States)] (ORCID:0000000338264397), Lu, Dongping [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000195978500), Hu, Enyuan [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000218814534), Meng, Y. Shirley [Univ. of California, San Diego, CA (United States)] (ORCID:0000000189368845), Wang, Chongmin [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)] (ORCID:0000000333270958), Liu, Jun [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)] (ORCID:0000000186637771), Zhang, Ji‐Guang [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000173434609), Xu, Wu [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000226858684). 2025-06-04. Designing Moderately‐Solvating Electrolytes for High‐Performance Lithium–Sulfur Batteries. https://doi.org/10.1002/adma.202503365

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