Electro‐Chemo‐Mechanical Modeling of Artificial Solid Electrolyte Interphase to Enable Uniform Electrodeposition of Lithium Metal Anodes (Adv. Energy Mater. 9/2022)

Liu, Yangyang; Xu, Xieyu; Kapitanova, Olesya O.; Евдокимов, П. В.; Song, Zhongxiao; Matic, Aleksandar; Xiong, Shizhao

doi:10.1002/aenm.202270035

Cited by 24 publications

(37 citation statements)

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“…As reported in our previous work, [ 40 ] the salt concentration of the electrolyte governs the mass transfer process of metal ions at the electrode surface of the metal plating as well as the ion depletion near the substrate—particularly for electrodeposition at high exchange current densities. Hence, tuning the concentration of the electrolyte (the DME:KFSI ratio in this study), can regulate the morphology of the electrodeposited K metal and even result in dendrite‐free electrodeposition.…”

Section: Resultsmentioning

confidence: 92%

High‐Energy and Long‐Lifespan Potassium–Sulfur Batteries Enabled by Concentrated Electrolyte

Lee

Park

Rizell

et al. 2022

Adv Funct Materials

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Potassium–sulfur (K–S) batteries are emerging as low‐cost and high‐capacity energy‐storage technology. However, conventional K–S batteries suffer from two critical issues that have not yet been successfully resolved: the dissolution of potassium polysulfides (KPS) into the liquid electrolyte and the formation of K dendrites on the K metal anode, which lead to inadequate cycling efficiencies with a low reversible capacity. Herein, a high‐capacity and long cycle‐life K–S battery consisting of a highly concentrated electrolyte (HCE) (4.34 mol kg−1 potassium bis(fluorosulfonyl)imide in a 1,2‐Dimethoxyethane) and a sulfurized polyacrylonitrile (SPAN) cathode is presented The application of a HCE efficiently suppresses the dendritic growth of K, as evidenced by operando optical imaging and phase field modeling, owing to the reduced K‐ion depletion on the electrode surface and a uniform Faradaic current density over the K metal anode surface. Additionally, because S is covalently bonded to the C backbone of PAN in the SPAN structure, the SPAN cathode inhibits the dissolution of KPS. These features generate synergy that the proposed K–S battery can provide a practical areal capacity of 2.5 mAh cm−2 and unprecedented lifetimes with high Coulombic efficiencies over 700 cycles.

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Section: Resultsmentioning

confidence: 92%

High‐Energy and Long‐Lifespan Potassium–Sulfur Batteries Enabled by Concentrated Electrolyte

Lee

Park

Rizell

et al. 2022

Adv Funct Materials

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“…[ 4,5 ] Nevertheless, the non‐uniform electrodeposition of Li metal during the charging process invariably leads to low Coulombic efficiency and growth of Li dendrites, hindering its commercialization in rechargeable batteries. [ 6–8 ]…”

Section: Introductionmentioning

confidence: 99%

Electro–Chemo–Mechanical Failure of Solid Electrolytes Induced by Growth of Internal Lithium Filaments

Liu

Kapitanova

et al. 2022

Advanced Materials

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vehicles, consumer electronics, and smart grid. [1] The pathway for gaining these targets is to build new battery chemistry by exploration of high-capacity anode and cathode materials as well as nonflammable electrolytes. [2,3] Metallic anodes, represented by lithium (Li), were the promising anode materials owing to their high theoretical capacity and it is, for instance, as high as 3860 mAh g −1 for Li-metal anodes. [4,5] Nevertheless, the non-uniform electrodeposition of Li metal during the charging process invariably leads to low Coulombic efficiency and growth of Li dendrites, hindering its commercialization in rechargeable batteries. [6][7][8] Utilization of solid electrolytes with high shear modulus was known as the most promising approach to suppress the formation of Li dendrites and to guarantee high safety of the battery at the same time. [9] Despite the significant advances aiming for high ionic conductivity of solid electrolytes, operation of solid-state batteries under the practical industry conditions, particularly for high-power systems, is not achieved yet. [10] A cell failure induced by the propagation of Li filaments (or Li dendrites) through solid electrolytes will be triggered once the applied current density is over a certain value which is defined as critical current density. [11] The growth of Li filaments leads to the failure of physical contact at interface, mechanical degradation of solid electrolyte, and even the short circuit of cell when the filaments connect the anode with cathode. [12] These failure processes have been reported for various solid electrolytes, including garnet Li 7 La 3 Zr 2 O 12 (LLZO), [13] amorphous 70Li 2 S-30P 2 S 5 glass, [14] argyrodite (Li 6 PS 5 Cl), [15] and sodium superionic conductor type (NASICON, such as Li 1+x Al x Ge 2−x (PO 4 ) 3 ). [16] Capturing the formation and the propagation of Li filaments in solid electrolyte to understand the failure mechanism of solid-state batteries is a great challenge since the microstructure evolution of interest is buried inside the solid electrolyte. [10] State of the art characterization techniques including operando synchrotron X-ray tomographic microscopy, [17] in situ transmission electron microscopy, [18] and operando neutron depth profiling [13] have been employed to track the internal evolution of solid electrolyte in real time by the combination of electrochemical methodologies. It is found that origin of Li filaments Growth of lithium (Li) filaments within solid electrolytes, leading to mechanical degradation of the electrolyte and even short circuit of the cell under high current density, is a great barrier to commercialization of solid-state Li-metal batteries. Understanding of this electro-chemo-mechanical phenomenon is hindered by the challenge of tracking local fields inside the solid electrolyte. Here, a multiphysics simulation aiming to investigate evolution of the mechanical failure of the solid electrolyte induced by the internal growth of Li is reported. Visualization of local stress, damage, and cra...

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“…[ 4,5 ] Nevertheless, Li metal tends to electrodeposit in dendrite‐form due to its ultrahigh exchange current density and repaid interfacial depletion of Li‐ion. As a Consequence, Li dendrites lead to a series of issues, [ 6–9 ] like short circuits, serious side reactions, increasing impedance, low Coulombic efficiency, etc., which impede the practical application of Li metal batteries. [ 10,11 ]…”

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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Electro‐Chemo‐Mechanical Modeling of Artificial Solid Electrolyte Interphase to Enable Uniform Electrodeposition of Lithium Metal Anodes (Adv. Energy Mater. 9/2022)

Cited by 24 publications

References 0 publications

High‐Energy and Long‐Lifespan Potassium–Sulfur Batteries Enabled by Concentrated Electrolyte

High‐Energy and Long‐Lifespan Potassium–Sulfur Batteries Enabled by Concentrated Electrolyte

Electro–Chemo–Mechanical Failure of Solid Electrolytes Induced by Growth of Internal Lithium Filaments

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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