Lithium-sulfur (Li-S) batteries are promising next-generation energy storage systems due to their ultrahigh theoretical energy density of 2600 Wh kg. However, soluble lithium polysulfides (LiPSs) violently corrode Li metal anodes, inducing rapid capacity decay and poor cycling lifespan of Li-S batteries. Herein, the corrosion of different LiPS species on the Li metal anode is systematically investigated.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2025
Coulombic efficiency (CE) is a quantifiable indicator for the reversibility of lithium metal anodes in high-energy-density batteries. However, the quantitative relationship between CE and electrolyte properties has yet to be established, impeding rational electrolyte design. Herein, an interpretable model for estimating CE based on data-driven insights of electrolyte properties is proposed.
View Article and Find Full Text PDFJ Am Chem Soc
May 2025
Lithium-sulfur (Li-S) batteries are promising in achieving high energy density but inferior in cycling lifespan since Li polysulfides (LiPSs) corrode Li metal anode. Weakening the electrolyte solvating power (ESP) for LiPSs effectively mitigates anodic corrosion but inevitably retards cathodic reaction kinetics. Herein, the correlation between the ESP and the LiPS redox kinetics in weakly solvating electrolyte is unveiled for achieving high-performance Li-S batteries.
View Article and Find Full Text PDFRenowned for their high theoretical energy density and cost-effectiveness, metal-sulfur (M-S) batteries are pivotal in overcoming the current energy storage bottlenecks and accelerating the transition toward a cleaner society. Polysulfides (PSs) serve as essential intermediates in M-S batteries and bridge the electrochemical redox processes of sulfur, playing a decisive role in controlling the electrode behaviors and regulating the battery performances. Understanding PS chemistry across diverse battery environments is key to advancing M-S batteries.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2024
Solid polymer electrolytes are promising electrolytes for safe and high-energy-density lithium metal batteries. However, traditional ether-based polymer electrolytes are limited by their low lithium-ion conductivity and narrow electrochemical window because of the well-defined and intimated Li-oxygen binding topologies in the solvation structure. Herein, we proposed a new strategy to reduce the Li-polymer interaction and strengthen the anion-polymer interaction by combining strong Li-O (ether) interactions, weak Li-O (ester) interactions with steric hindrance in polymer electrolytes.
View Article and Find Full Text PDFLithium-sulfur (Li-S) batteries are highly considered as next-generation energy storage techniques. Weakly solvating electrolyte with low lithium polysulfide (LiPS) solvating power promises Li anode protection and improved cycling stability. However, the cathodic LiPS kinetics is inevitably deteriorated, resulting in severe cathodic polarization and limited energy density.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2024
The cycle life of high-energy-density lithium-sulfur (Li-S) batteries is severely plagued by the incessant parasitic reactions between Li metal anodes and reactive Li polysulfides (LiPSs). Encapsulating Li-polysulfide electrolyte (EPSE) emerges as an effective electrolyte design to mitigate the parasitic reactions kinetically. Nevertheless, the rate performance of Li-S batteries with EPSE is synchronously suppressed.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2023
Lithium-sulfur (Li-S) batteries are promising due to ultrahigh theoretical energy density. However, their cycling lifespan is crucially affected by the electrode kinetics of lithium polysulfides. Herein, the polysulfide solvation structure is correlated with polysulfide electrode kinetics towards long-cycling Li-S batteries.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2023
The stability of high-energy-density lithium metal batteries depends on the uniformity of solid electrolyte interphase (SEI) on lithium metal anodes. Rationally improving SEI uniformity is hindered by poorly understanding the effect of structure and components of SEI on its uniformity. Herein, a bilayer structure of SEI formed by isosorbide dinitrate (ISDN) additives in localized high-concentration electrolytes was demonstrated to improve SEI uniformity.
View Article and Find Full Text PDFLithium-sulfur (Li-S) batteries afford great promise on achieving practical high energy density beyond lithium-ion batteries. Lean-electrolyte conditions constitute the prerequisite for achieving high-energy-density Li-S batteries but inevitably deteriorates battery performances, especially the sulfur cathode kinetics. Herein, the polarizations of the sulfur cathode are systematically decoupled to identify the key kinetic limiting factor in lean-electrolyte Li-S batteries.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2023
Practical lithium-sulfur (Li-S) batteries are severely plagued by the instability of solid electrolyte interphase (SEI) formed in routine ether electrolytes. Herein, an electrolyte with 1,3,5-trioxane (TO) and 1,2-dimethoxyethane (DME) as co-solvents is proposed to construct a high-mechanical-stability SEI by enriching organic components in Li-S batteries. The high-mechanical-stability SEI works compatibly in Li-S batteries.
View Article and Find Full Text PDFLithium-sulfur (Li-S) batteries are regarded as promising high-energy-density energy storage devices. However, the cycling stability of Li-S batteries is restricted by the parasitic reactions between Li metal anodes and soluble lithium polysulfides (LiPSs). Encapsulating LiPS electrolyte (EPSE) can efficiently suppress the parasitic reactions but inevitably sacrifices the cathode sulfur redox kinetics.
View Article and Find Full Text PDFBackground: Transjugular intrahepatic portosystemic shunt (TIPS) is placed important role in the therapy of complications of portal hypertension, there is still no suitable criterion for a reduction in portosystemic gradient (PSG), which can both reduce PSG and maximize clinical results and minimize hepatic encephalopathy (HE).
Aim: To compare the clinical outcomes and incidence of HE after one-third PSG reduction during TIPS in patients with variceal bleeding and refractory ascites.
Methods: A total of 1280 patients with portal-hypertension-related complications of refractory ascites or variceal bleeding who underwent TIPS from January 2016 to January 2019 were analyzed retrospectively.
In recent years, the rapid development of modern society is calling for advanced energy storage to meet the growing demands of energy supply and generation. As one of the most promising energy storage systems, secondary batteries are attracting much attention. The electrolyte is an important part of the secondary battery, and its composition is closely related to the electrochemical performance of the secondary batteries.
View Article and Find Full Text PDFFundam Res
November 2024
Lithium metal is one of the most promising anode materials for next-generation high-energy-density rechargeable batteries. A fundamental mechanism understanding of the dead lithium formation under the interplay of electrochemistry and mechanics in lithium metal batteries is strongly considered. Herein, we proposed a mechano-electrochemical phase-field model to describe the lithium stripping process and quantify the dead lithium formation under stress.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2022
Advanced electrolyte design is essential for building high-energy-density lithium (Li) batteries, and introducing anions into the Li solvation sheaths has been widely demonstrated as a promising strategy. However, a fundamental understanding of the critical role of anions in such electrolytes is very lacking. Herein, the anionic chemistry in regulating the electrolyte structure and stability is probed by combining computational and experimental approaches.
View Article and Find Full Text PDFLithium (Li)-metal batteries promise energy density beyond 400 Wh kg , while their practical operation at an extreme temperature below -30 °C suffers severe capacity deterioration. Such battery failure highly relates to the remarkably increased kinetic barrier of interfacial processes, including interfacial desolvation, ion transportation, and charge transfer. In this work, the interfacial kinetics in three prototypical electrolytes are quantitatively probed by three-electrode electrochemical techniques and molecular dynamics simulations.
View Article and Find Full Text PDFLong cycling lifespan is a prerequisite for practical lithium-sulfur batteries yet is restricted by side reactions between soluble polysulfides and the lithium-metal anode. The regulation on solvation structure of polysulfides renders encapsulating polysulfides electrolytes (EPSE) as a promising solution to suppress the parasitic reactions. The solvating power of the solvents in the outer solvent shell of lithium polysulfides is critical for the encapsulation effect of EPSE.
View Article and Find Full Text PDFThe life span of lithium batteries as energy storage devices is plagued by irreversible interfacial reactions between reactive anodes and electrolytes. Occurring on polycrystal surface, the reaction process is inevitably affected by the surface microstructure of anodes, of which the understanding is imperative but rarely touched. Here, the effect of grain boundary of lithium metal anodes on the reactions was investigated.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2022
The performance of rechargeable lithium (Li) batteries is highly correlated with the structure of solid electrolyte interphase (SEI). The properties of a working anode are vital factors in determining the structure of SEI; however, the correspondingly poor understanding hinders the rational regulation of SEI. Herein, the electrode potential and anode material, two critical properties of an anode, in dictating the structural evolution of SEI were investigated theoretically and experimentally.
View Article and Find Full Text PDFLithium-sulfur (Li-S) batteries have great potential as high-energy-density energy storage devices. Electrocatalysts are widely adopted to accelerate the cathodic sulfur redox kinetics. The interactions among the electrocatalysts, solvents, and lithium salts significantly determine the actual performance of working Li-S batteries.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2022
The lifespan of practical lithium (Li)-metal batteries is severely hindered by the instability of Li-metal anodes. Fluorinated solid electrolyte interphase (SEI) emerges as a promising strategy to improve the stability of Li-metal anodes. The rational design of fluorinated molecules is pivotal to construct fluorinated SEI.
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