The shuttling phenomena in lithium-sulfur batteries lead to drastic attenuation of the capacity. This can be suppressed effectively by modifying the separator. Herein, a double-layered separator composed of a macroporous polypropylene (PP) matrix layer and an arrayed poly(methyl methacrylate) (PMMA) microsphere retarding layer is designed as the separator for lithium-sulfur batteries. A sulfur positive electrode with the PP/PMMA separator exhibits a high initial capacity of 1100.10 mAh g at a current density of 0.1 mA cm along with a high Coulombic efficiency, which is higher than the corresponding first discharge capacity results obtained using the standard PP separator (948.60 mAh g). In the double-layered separator, the arrayed PMMA microspheres can inhibit the diffusion of polysulfides through physical and chemical adsorption, thereby improving the electrochemical performance of lithium-sulfur batteries. In addition, the PMMA microspheres enhance the affinity of the separator to the electrolyte, which will increase the adsorption of the electrolyte to the separator and accelerate the diffusion rate of lithium ions.
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http://dx.doi.org/10.1021/acsami.8b14196 | DOI Listing |
Adv Sci (Weinh)
December 2024
Key Laboratory for Photonic and Electronic Bandgap Materials, Ministry of Education, School of Physics and Electronic Engineering, Harbin Normal University, Harbin, Heilongjiang, 150025, China.
Lithium-sulfur batteries (LSBs) offer high energy density and environmental benefits hampered by the shuttle effect related to sluggish redox reactions of long-chain lithium polysulfides (LiPSs). However, the fashion modification of the d-band center in separators is still ineffective, wherein the mechanism understanding always relies on theoretical calculations. This study visibly probed the evolution of the Co 3d-band center during charge and discharge using advanced inverse photoemission spectroscopy/ultraviolet photoemission spectroscopy (IPES/UPS), which offers reliable evidence and are consistent well with theoretical calculations.
View Article and Find Full Text PDFChemistry
December 2024
Dalian University of Technology, No.2 Linggong Road, Ganjingzi District, Dalian, CHINA.
Sulfur-rich copolymers have gained a great deal of attention as promising cathode materials in Li-S batteries due to their low cost and naturally uniform sulfur dispersion. However, the poor electrical conductivity and shuttle effect cause rapid capacity decay and low sulfur utilization especially under high sulfur loading and low electrolyte/sulfur ratio. Herein, the Fe1-xS/C dispersed and Se-containing sulfur-rich polymer (FSP) was synthesized by one-pot reaction of ferrocene, trithioiynuric acid with SexSy.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Henan University, School of Materials Science and Engineering, CHINA.
Sluggish reaction kinetics of sulfur species fundamentally trigger the incomplete conversion of S8↔Li2S and restricted lifespan of lithium-sulfur batteries, especially under high sulfur loading and/or low electrolyte/sulfur (E/S) ratio. Introducing redox mediators (RMs) is an effective strategy to boost the battery reaction kinetics, yet their multifunctionality and shuttle inhibition are still not available. Here, a unique ethyl viologen (EtV²⁺) RM with two highly reversible redox couples (EtV²⁺/EtV⁺, EtV⁺/EtV0) is demonstrated to well match the redox chemistry of sulfur species, in terms of accelerating the electron transfer in S8 reduction, Li2S nucleation and the Li2S oxidation.
View Article and Find Full Text PDFSmall
December 2024
School of Materials science and Engineering, Zhengzhou University, Zhengzhou, 450001, China.
The mesopores and macropores within porous carbon materials help increase the surface for the depostion of solid-state products, reduce the LiS film thickness, enhance electron and mass transport, and accelerate the reaction kinetics. However, an excessive amount of mesopores and macropores can lead to increased electrolyte consumption, particularly at high sulfur loadings, where excessive electrolyte usage hampers the enhancement of practical energy density in lithium-sulfur (Li-S) batteries. A rational pore structure can minimize the amount of electrolyte to fill the pores, thereby reducing electrolyte consumption while achieving rapid reaction kinetics and a high gravimetric energy density.
View Article and Find Full Text PDFSmall
December 2024
School of Physical Science and Technology, Lanzhou University, 222 South Tianshui Road, Lanzhou, 730000, China.
Well-designed structures of the electrocatalyst provide excellent catalytic activity and high structural stability during the sulfur reduction reaction of Lithium-sulfur batteries (LSBs). In this study, a novel and efficient structure is developed to encapsulate bimetallic FeCo nanoalloy catalysts within N-doped carbon nanotube (NCNT) on carbon nanofibers (FeCo@NCNT/CNFs) using a combination of electrospinning and rapid-cooling techniques. The NCNT matrix with abundant sites not only serves as a high pathway for electron transport during the reaction, but its encapsulation structure also acts as armor to protect the FeCo nanoalloy.
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