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Lithium-sulfur (Li-S) batteries have arousing interest because of their high theoretical energy density. However, they often suffer from sluggish conversion of lithium polysulfides (LiPS) during the charge/discharge process. Single nickel (Ni) atoms on nitrogen-doped graphene (Ni@NG) with Ni-N structure are prepared and introduced to modify the separators of Li-S batteries. The oxidized Ni sites of the Ni-N structure act as polysulfide traps, efficiently accommodating polysulfide ion electrons by forming strong S ⋅⋅⋅NiN bonding. Additionally, charge transfer between the LiPS and oxidized Ni sites endows the LiPS on Ni@NG with low free energy and decomposition energy barrier in an electrochemical process, accelerating the kinetic conversion of LiPS during the charge/discharge process. Furthermore, the large binding energy of LiPS on Ni@NG also shows its ability to immobilize the LiPS and further suppresses the undesirable shuttle effect. Therefore, a Li-S battery based on a Ni@NG modified separator exhibits excellent rate performance and stable cycling life with only 0.06% capacity decay per cycle. It affords fresh insights for developing single-atom catalysts to accelerate the kinetic conversion of LiPS for highly stable Li-S batteries.
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http://dx.doi.org/10.1002/adma.201903955 | DOI Listing |
Adv Mater
September 2025
School of Materials Science and Chemical Engineering, Harbin University of Science and Technology, Harbin, 150080, China.
The polysulfide shuttling and sluggish sulfur redox kinetics hinder the commercialization of lithium-sulfur (Li-S) batteries. Herein, the fabrication of phosphorus (P)-doped iron telluride (FeTe) nanoparticles with engineered Te vacancies anchored on nitrogen (N)-doped carbon (C) (P-FeTe@NC) is presented as a multifunctional sulfur host. Theoretical and experimental analyses show that Te vacancies create electron-deficient Fe sites, which chemically anchor polysulfides through enhanced Fe─S covalent interactions.
View Article and Find Full Text PDFACS Sustain Chem Eng
September 2025
Electrochemical Innovation Lab, Department of Chemical Engineering, University College London, Torrington Place, London WC1E 7JE, U.K.
Traditionally, binders such as poly-(vinylidene fluoride) (PVDF) have been used within lithium-sulfur (Li-S) batteries, but these present environmental and recyclability challenges and have little to no impact on the processes that drive degradation in the cell's chemistry. Ideally, a Li-S battery binder would contribute to the mitigation of the polysulfide shuttle effect and negate the impacts of positive electrode volume expansion while being compatible with aqueous ink preparation and low-energy, low-toxicity recycling processes. In this work, we demonstrate that fibroin, an economical and sustainable biological polymer with an abundance of functional groups, can effectively trap polysulfides while still offering the durability, cyclability, and ease of use offered by the current state-of-the-art binder (PVDF).
View Article and Find Full Text PDFJ Colloid Interface Sci
August 2025
Materials Institute of Atomic and Molecular Science, Shaanxi University of Science and Technology, Xi'an 710021, China. Electronic address:
The commercialization of lithium‑sulfur (LiS) batteries faces fundamental issues from polysulfide shuttling to inefficient redox kinetics, compounded by the absence of systematic methods for catalyst design. Herein, we present a machine learning (ML)-driven strategy to design MoS/MoO heterostructures anchored on nitrogen-doped hollow carbon shells (NCS) via gradient boosting decision trees modeling. The ML-guided optimization identifies critical synthesis parameters (e.
View Article and Find Full Text PDFLangmuir
September 2025
High Energy Density Batteries Research Laboratory, Department of Physics, Pondicherry University, Puducherry 605014, India.
Lithium-sulfur batteries have attracted significant attention recently as sulfur is one of the most abundant elements in the earth's crust, low-cost, has a non-toxic nature, multi-electron transfer property coupled with its remarkable theoretical specific capacity of 1672 mAh g and energy density of 2600 Wh kg. However, lithium-deficient sulfur cathodes associated with lithium metal anodes together to face challenges, such as significant volume expansion during cycling, dendrite formation, and polysulfide shuttling effect from the sulfur cathodes, leading to corrosion, all of which negatively impact the cycle lifespan of the battery. On the other hand, moving away from liquid to solid-state garnet-based solid electrolytes is highly aided for lithium-sulfur batteries because of their high ionic conductivity of 10 S cm stability with lithium metal, lithium-based alloys and moreover in mitigating the polysulfide issues.
View Article and Find Full Text PDFACS Nano
September 2025
Faculty of Materials Science and Energy Engineering, Shenzhen University of Advanced Technology, Shenzhen 518107, China.
The variable valence states of iodine(I) render Zn-I batteries an intriguing area of research. However, current Zn-I batteries are mostly based on I/I redox chemistry. Effective strategies for activating the high-voltage I/I redox couple in iodine-based cathode materials remain relatively scarce.
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