Lithium-sulfur (Li-S) batteries are candidates for next-generation energy storage systems because of their low cost, high theoretical specific capacity and safety. However, the serious lithium polysulfide (LiPS) shuttle effect leads to a loss of reactive active substances and reduction of coulombic efficiency. In the current work, iron oxide (IO-700)-prepared by calcining a mixture of carbon spheres and ferric nitrate under an air atmosphere at 700 °C-was designed as a separator modifier to effectively adsorb LiPSs and accelerate the kinetics of the transformation of the intermediates, thereby inhibiting the shuttle effect. Li-S batteries including IO-700 showed long-term stability for 1000 cycles at 1C, with a capacity decay rate per cycle of only 0.0487%. A theoretical calculation indicated that, due to strongly polar active sites, FeO adsorbed LiPSs effectively to suppress the shuttle effect. This work has highlighted the importance for Li-S batteries of strongly polar active sites for anchoring LiPSs to inhibit the shuttle effect.
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http://dx.doi.org/10.1039/d2cc06893a | DOI Listing |
Nanomaterials (Basel)
December 2024
State Key Laboratory of Heavy Oil Processing, Institute of New Energy, College of New Energy, China University of Petroleum (East China), Qingdao 266580, China.
The integration of intermittent renewable energy sources into the energy supply has driven the need for large-scale energy storage technologies. Vanadium redox flow batteries (VRFBs) are considered promising due to their long lifespan, high safety, and flexible design. However, the graphite felt (GF) electrode, a critical component of VRFBs, faces challenges due to the scarcity of active sites, leading to low electrochemical activity.
View Article and Find Full Text PDFACS Nano
December 2024
College of Energy, Soochow Institute for Energy and Materials Innovations, Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Soochow University, Suzhou 215006, China.
The adsorption-conversion paradigm of polysulfides during the sulfur reduction reaction (SRR) is appealing to tackle the shuttle effect in Li-S batteries, especially based upon atomically dispersed electrocatalysts. However, mechanistic insights into such catalytic systems remain ambiguous, limiting the understanding of sulfur electrochemistry and retarding the rational design of available catalysts. Herein, we systematically explore the polysulfide adsorption-conversion essence via a geminal-atom model system to understand the catalyst roles toward an expedited SRR.
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 PDFAngew Chem Int Ed Engl
December 2024
Huazhong University of Science and Technology - Main Campus: Huazhong University of Science and Technology, Materials Science and Engineering, CHINA.
Sulfurized polyacrylonitrile (SPAN) presents an opportunity to replace elemental sulfur as a "shuttle-free" cathode for secondary Li-S batteries, which can be an ideal choice for stationary energy storage due to its abundance, low cost, and sustainability. The electrolyte options for the state-of-the-art SPAN batteries have been limited to the flammable carbonate and ether ones, which raises safety concerns. Here, we explored the use of a non-flammable acetonitrile (AN) electrolyte for SPAN battery for the first time and identified the irreversible cleavage of C-S bonds of SPAN as the main reason for the failure of SPAN in AN electrolyte.
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