The sluggish kinetics of lithium-sulfur (Li-S) batteries severely impedes the application in extreme conditions. Bridging the sulfur cathode and lithium anode, the electrolyte plays a crucial role in regulating kinetic behaviors of Li-S batteries. Herein, we report a multifunctional electrolyte additive of phenyl selenium bromide (PhSeBr) to simultaneously exert positive influences on both electrodes and the electrolyte. For the cathode, an ideal conversion routine with lower energy barrier can be attained by the redox mediator and homogeneous catalyst derived from PhSeBr, thus improving the reaction kinetics and utilization of sulfur. Meanwhile, the presence of Se-Br bond helps to reconstruct a loose solvation sheath of lithium ions and a robust bilayer SEI with excellent ionic conductivity, which contributes to reducing the de-solvation energy and simultaneously enhancing the interfacial kinetics. The Li-S battery with PhSeBr displays superior long cycling stability with a reversible capacity of 1164.7 mAh g after 300 cycles at 0.5 C rate. And the pouch cell exhibits a maximum capacity of 845.3 mAh and a capacity retention of 94.8 % after 50 cycles. Excellent electrochemical properties are also obtained in extreme conditions of high sulfur loadings and low temperature of -20 °C. This work demonstrates the versatility and practicability of the special additive, striking out an efficient but simple method to design advanced Li-S batteries.
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http://dx.doi.org/10.1002/anie.202405880 | DOI Listing |
Small Methods
January 2025
School of Materials Science and Engineering, Central South University, Changsha, Hunan, 410083, P. R. China.
Alluaudite-type NaFe(SO) (NFS) with high theoretical energy density is regarded as the promising cathode of sodium-ion batteries (SIBs), while practical rate and cyclic performances are still hindered by intrinsic poor conductivity. Here, a facile method is developed, collaborating high-boiling organic solvents assisted colloidal synthesis (HOS-CS) with sintering for tailoring NaFe(SO) nanocrystals decorated by conductive carbon network toward high-rate-capability cathode of SIBs. Impressively, the as-prepared NaFe(SO)@MC provides 60.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Energy Research Institute@NTU (ERI@N), Interdisciplinary Graduate Programme, Nanyang Technological University, Singapore639798 ,Singapore.
Understanding the structure-property relationship and the way in which catalysts facilitate polysulfide conversion is crucial for the rational design of lithium-sulfur (Li-S) battery catalysts. Herein, a series of NiAlO, CoAlO, and CuAlO spinel oxides with varying Ni, Co, or Cu tetrahedral and octahedral site occupancy are studied as Li-S battery catalysts. Combined with experimental and theoretical analysis, the tetrahedral site is identified as the most active site for enhancing polysulfide adsorption and charge transfer.
View Article and Find Full Text PDFMolecules
December 2024
Shanxi Key Laboratory of Carbon Materials, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China.
Lithium-sulfur (Li-S) batteries have emerged as a promising candidate for next-generation high-energy rechargeable lithium batteries, but their practical application is impeded by the sluggish redox kinetics and low sulfur loading. Here, we report the in situ growth of δ-MnO nanosheets onto hierarchical porous carbon microspheres (HPCs) to form an HPCs/S@MnO composite for advanced lithium-sulfur batteries. The delicately designed hybrid architecture can effectively confine LiPSs and obtain high sulfur loading up to 10 mg cm, in which the inner carbon microspheres with a large pore volume and large specific surface area can encapsulate high sulfur content, and the outer MnO nanosheets, as a catalytic layer, can improve the conversion reaction of LiPSs and suppress the shuttle effect.
View Article and Find Full Text PDFNat 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 PDFChem Commun (Camb)
January 2025
Institute for Carbon Neutralization Technology, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang 325035, China.
Single-atom catalysts (SACs) have become the forefront and hotspot in energy storage and conversion research, inheriting the advantages of both homogeneous and heterogeneous catalysts. In particular, carbon-supported SACs (CS-SACs) are excellent candidates for many energy storage and conversion applications, due to their maximum atomic efficiency, unique electronic and coordination structures, and beneficial synergistic effects between active catalytic sites and carbon substrates. In this review, we briefly review the atomic-level regulation strategies for optimizing CS-SACs for energy storage and conversion, including coordination structure control, nonmetallic elemental doping, axial coordination design, and polymetallic active site construction.
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