The development of all-solid-state lithium-sulfur batteries (ASSLSBs) toward large-scale electrochemical energy storage is driven by the higher specific energies and lower cost in comparison with the state-of-the-art Li-ion batteries. Yet, insufficient mechanistic understanding and quantitative parameters of the key components in sulfur-based cathode hinders the advancement of the ASSLSB technologies. This review offers a comprehensive analysis of electrode parameters, including specific capacity, voltage, S mass loading and S content toward establishing the specific energy (Wh kg) and energy density (Wh L) of the ASSLSBs. Additionally, this work critically evaluates the progress in enhancing lithium ion and electron percolation and mitigating electrochemical-mechanical degradation in sulfur-based cathodes. Last, a critical outlook on potential future research directions is provided to guide the rational design of high-performance sulfur-based cathodes toward practical ASSLSBs.
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http://dx.doi.org/10.1002/adma.202407738 | DOI Listing |
Nat Mater
January 2025
Department of Mechanical Engineering, The Pennsylvania State University, University Park, PA, USA.
Lithium-sulfur (Li-S) all-solid-state batteries (ASSBs) hold great promise for next-generation safe, durable and energy-dense battery technology. However, solid-state sulfur conversion reactions are kinetically sluggish and primarily constrained to the restricted three-phase boundary area of sulfur, carbon and solid electrolytes, making it challenging to achieve high sulfur utilization. Here we develop and implement mixed ionic-electronic conductors (MIECs) in sulfur cathodes to replace conventional solid electrolytes and invoke conversion reactions at sulfur-MIEC interfaces in addition to traditional three-phase boundaries.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Department of Physics and Astronomy, Clemson University, Clemson, South Carolina 29634, United States.
Solid-state lithium-sulfur (Li-S) batteries show promise for future electric mobility due to their high energy density potential. However, high internal impedance, Li polysulfide shuttling, and dendrite formation exist. Herein, we present a Li-rich cellulosic solid-state electrolyte (SSE) that, when paired with a sulfurized polyacrylonitrile (SPAN) cathode, leads to durable Li-S batteries for use in the room temperature to 50 °C range.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
State Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China.
Using a solid electrolyte is considered to be the most effective strategy to solve the shuttle effect in lithium-sulfur batteries. However, the practical application of solid-state lithium-sulfur batteries (SLSBs) is still far from being realized. This is because SLSBs, like all other solid-state battery systems, also face the dilemma of interface degradation (including both the anode and cathode interfaces), in addition to terrible kinetics due to the nonliquid solid-state electrolytes infiltrating the nonconductive sulfur particles inside the cathode.
View Article and Find Full Text PDFJ Am Chem Soc
December 2024
Shenzhen Geim Graphene Center, Shenzhen Key Laboratory for Graphene-based Materials, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China.
Poly(ethylene oxide) (PEO)-based solid-state lithium-sulfur batteries (SSLSBs) have garnered considerable interest owing to their impressive energy density and high safety. However, the dissolved lithium polysulfide (LiPS) together with sluggish reaction kinetics disrupts the electrolyte network, bringing about ionic conductive breakpoints and severely limiting battery performance. To cure this, we propose an in situ welding strategy by introducing phosphorus pentasulfide (PS) as the welding filler into PEO-based solid cathodes.
View Article and Find Full Text PDFChem Commun (Camb)
December 2024
Energy Storage Research Center, Korea Institute of Science and Technology, Seoul 02792, Republic of Korea.
We reveal the reversible redox mechanism of LiPSCl in composite cathodes for practical all-solid-state lithium-sulfur batteries. The limited electrochemical reactivity of the non-conducting sulfur-based active material induces the formation of LiPSCl decomposition products, which allows the recrystallization of LiPSCl through a reversible redox process, contributing to the composite cathode capacity.
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