Promoted rate and cycling capability of Li–S batteries enabled by targeted selection of co-solvent for the electrolyte

Liu, Yangyang; Pan, Yi-Zhen; Ban, Jun; Li, Tongtong; Jiao, Xingxing; Hong, Xiaobin; Xie, Kai; Song, Jiangxuan; Matic, Aleksandar

doi:10.1016/j.ensm.2019.10.022

Cited by 26 publications

(20 citation statements)

References 44 publications

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“…These days, tremendous endeavor has been devoted to suppressing the non‐uniform electrodeposition of dendritic Li, stabilizing the interface with electrolyte, and guaranteeing the cyclic performance of LMBs. [ 3a,7 ] The advanced strategies including optimization of electrolytes like additives and solvent selection, [ 8 ] artificial solid electrolyte interphase (SEI) with multifunctional properties, [ 9 ] solid‐state electrolyte, [ 10 ] and functionalized separator, [ 11 ] have been reported. These approaches can improve the stability of Li metal anode to a certain extent, which is confirmed by the smooth morphology of cycled Li anode and the prolonged cyclic life.…”

Section: Introductionmentioning

confidence: 99%

Diffusion Limited Current Density: A Watershed in Electrodeposition of Lithium Metal Anode

Jiao

Kapitanova

et al. 2022

Advanced Energy Materials

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Lithium metal is considered to be a promising anode material for high‐energy‐density rechargeable batteries because of its high theoretical capacity and low reduction potential. Nevertheless, the practical application of Li anodes is challenged by poor cyclic performance and potential safety hazards, which are attributed to non‐uniform electrodeposition of Li metal during charging. Herein, diffusion limited current density (DLCD), one of the critical fundamental parameters that govern the electrochemical reaction process, is investigated as the threshold of current density for electrodeposition of Li. The visualization of the concentration field and distribution of Faradic current density reveal how uniform electrodeposition of Li metal anodes can be obtained when the applied current density is below the DLCD of the related electrochemical system. Moreover, the electrodeposition of Li metal within broken solid electrolyte interphases preferentially occurs at the crack spots that are caused by the non‐uniform electrodeposition of Li metal. This post‐electrodeposition leads to more consumption of active Li when the applied current density is greater than the DLCD. Therefore, lowering the applied current density or increasing the DLCD are proposed as directions for developing advanced strategies to realize uniform electrodeposition of Li metal and stable interfaces, aiming to accelerate the practical application of state‐of‐the‐art Li metal batteries.

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Section: Introductionmentioning

confidence: 99%

Diffusion Limited Current Density: A Watershed in Electrodeposition of Lithium Metal Anode

Jiao

Kapitanova

et al. 2022

Advanced Energy Materials

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“…Due to this diffusion of polysulfides, attention must be paid to the carbonsulfur cathode microstructure and the effects this will have on cell performance. [9,10] Moreover, the end-product Li 2 S has a low solubility in commonly used liquid electrolytes [11,12] and, as soon as it is formed, it precipitates as insulating Li 2 S on the cathode surface. Generally, these phenomena lead to a poor utilization of the active material, limiting the specific capacity of LiS cells.…”

Section: Introductionmentioning

confidence: 99%

Visualization of Dissolution‐Precipitation Processes in Lithium–Sulfur Batteries

Sadd

Angelis

Colding‐Jørgensen

et al. 2022

Advanced Energy Materials

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of state-of-the-art cathodic materials in Li-ion cells. Furthermore, in contrast to materials in standard intercalation-based electrodes, [2] sulfur is highly abundant, [3] has a low cost, and is non-toxic. [3,4] Considering also that a typical sulfur composite cathode contains only sulfur, carbon, and binder, these metrics bear the promise of a sustainable, cost-effective, and high energy density next-generation energy storage technology.The high specific capacity stems from the conversion reaction where elemental sulfur (S 8 ) is converted to lithium sulfide (Li 2 S) during discharge. The conversion mechanism is complex and multiple reaction pathways have been proposed. [5,6] Common to the different pathways is that it takes place through a series of soluble intermediate polysulfide species (Li 2 S n ), where the specific speciation can vary with, for example, electrolyte composition and amount, or operating conditions. Irrespective of pathway, the conversion process leads to several challenges in the realization of practical high energy density LiS cells. [4,[6][7][8] Polysulfides created during the electrochemical conversion are highly soluble in common liquid electrolytes and their presence in the liquid phase leads to their In this work, light is shed on the dissolution and precipitation processes S8 and Li 2 S, and their role in the utilization of active material in LiS batteries. Combining operando X-ray Tomographic Microscopy and optical image analysis, in real-time; sulfur conversion/dissolution in the cathode, the diffusion of polysulfides in the bulk electrolyte, and the redeposition of the product of the electrochemical reaction, Li 2 S, on the cathode are followed. Using a customdesigned capillary cell, positioning the entire cathode volume within the field of view, the conversion of elemental sulfur to soluble polysulfides during discharge is quantitatively followed. The results show the full utilization of elemental sulfur in the cathode in the initial stage of discharge, with all solid sulfur converted to soluble polysulfide species. Optical image analysis shows a rapid diffusion of polysulfides as they migrate from the cathode to the bulk electrolyte at the start of discharge and back to the cathode in the later stages of discharge, with the formation and precipitation of Li 2 S. The results point to the redeposition of Li 2 S on all available surfaces in the cathode forming a continuous insulating layer, leaving polysulfide species remaining in the electrolyte, and this is the process limiting the cell's specific capacity.

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“…As a Consequence, Li dendrites lead to a series of issues, [6][7][8][9] like short circuits, serious side reactions, increasing impedance, low Coulombic efficiency, etc., which impede the practical application of Li metal batteries. [10,11] Recently, plenty of effective strategies have been proposed to suppress the growth of Li dendrites, [12] including structural and componential design of anode, [13,14] stabilization of interphase with artificial solid electrolyte interphase, [15,16] and optimization of electrolytes, [17][18][19] as well as separator modification. [20,21] Among myriad approaches, the surface modification of the anode with a functional coating is regarded as the effective strategy to realize uniform electrodeposition of Li metal and to settle the issues caused by the dendritic Li growth, including copper nitride, [22] titania, and aluminum oxide [23] embraced in polyacrylonitrile and other polymer-based composites.…”

Section: Introductionmentioning

confidence: 99%

Two Birds with One Stone: Using Indium Oxide Surficial Modification to Tune Inner Helmholtz Plane and Regulate Nucleation for Dendrite‐free Lithium Anode

Chen

Gao

et al. 2022

Small Methods

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Lithium metal has been considered as the most promising anode material due to its distinguished specific capacity of 3860 mAh g–1 and the lowest reduction potential of ‐3.04 V versus the Standard Hydrogen Electrode. However, the practicalization of Li‐metal batteries (LMBs) is still challenged by the dendritic growth of Li during cycling, which is governed by the surface properties of the electrodepositing substrate. Herein, a surface modification with indium oxide on the copper current collector via magnetron sputtering, which can be spontaneously lithiated to form a composite of lithium indium oxide and Li‐In alloy, is proposed. Thus, the growth of Li dendrites is effectively suppressed via regulating the inner Helmholtz plane modified with LiInO2 to foster the desolvation of Li‐ion and induce the nucleation of Li‐metal in two‐dimensions through electro‐crystallization with Li‐In alloy. Using the In2O3 modification, the Li‐metal anode exhibits outstanding cyclic stability, and LMBs with lithium cobalt oxide cathode present excellent capacity retention (above 80% over 600 cycles). Enlightening, the scalable magnetron sputtering method reported here paves a novel way to accelerate the practical application of the Li anode in LMBs to pursue higher energy density.

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Promoted rate and cycling capability of Li–S batteries enabled by targeted selection of co-solvent for the electrolyte

Cited by 26 publications

References 44 publications

Diffusion Limited Current Density: A Watershed in Electrodeposition of Lithium Metal Anode

Diffusion Limited Current Density: A Watershed in Electrodeposition of Lithium Metal Anode

Visualization of Dissolution‐Precipitation Processes in Lithium–Sulfur Batteries

Two Birds with One Stone: Using Indium Oxide Surficial Modification to Tune Inner Helmholtz Plane and Regulate Nucleation for Dendrite‐free Lithium Anode

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