A Perspective on interfacial engineering of lithium metal anodes and beyond

Yan, Qizhang; Whang, Grace; Wei, Ziyang; Ko, Shu-Ting; Sautet, Philippe; Tolbert, Sarah H.; Dunn, Bruce; Luo, Jian

doi:10.1063/5.0018417

Cited by 21 publications

(18 citation statements)

References 108 publications

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“…[8a,10] Also, these lithium alloys usually possess large chemical diffusion coefficient, which decreases the energy barrier of Li diffusing and spontaneously drives the fast lithium transfer from Li-rich phase to Li-poor phase. [11] Hence, molten Li can easily spread on the surface of these lithium alloys and form a homogeneous lithium layer. From this respect, a thin lithiophilic metal interphase with good contact with the substrate may be a good choice to realize close contact between metallic Li and Cu foil.…”

Section: Introductionmentioning

confidence: 99%

Doctor‐Blade Casting Fabrication of Ultrathin Li Metal Electrode for High‐Energy‐Density Batteries

Wang

Wan

et al. 2021

Advanced Energy Materials

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3860 mA h g −1 for metallic Li versus 372 mA h g −1 for graphite) and lowest redox voltage (−3.04 V versus standard hydrogen electrode) among all the anodes, exhibiting great promise as high-performance anode in the next-generation highenergy-density lithium-based rechargeable batteries. [3] Nevertheless, nearly infinite volume expansion/shrinkage and inhomogeneous stripping/plating behavior lead to the growth of dendritic behaviors of metallic Li, which would cause short circuits and other safety issues. [3b,4] Accompanied by large volume change, repeated fracture and repair of solid electrolyte interface (SEI) occurs during the charge/ discharge processes, which causes continuous consumption of active lithium and electrolyte, and finally inferior cycling stability. [5] Recently, extensive studies on electrode surface protection, composite structure, and electrolyte engineering have been conducted to improve the cycle life and safety hazards of metallic Li electrode. [6] However, highly overloaded lithium metal anodes (e.g., 500 µm for ≈100 mA h cm −2 ) and flooding amount of electrolytes were often employed for the evaluation of electrochemical performance of metallic Li. The use of thick Li metal anodes and excessive electrolyte does not support high energy density of batteries and are not feasible in practical applications. Therefore, high-performance ultrathin lithium metal anodes (e.g., 10-50 µm) that possess matched capacities with current cathodes are of key importance to practical battery application. However, the high homologous temperature (T h , for metallic lithium, T h is 0.66 at room temperature) of metallic Li at room temperature leads a strong influence of diffusion creep on its deformation, [7] and the resulting sticky nature and poor mechanical processability make it challenging to realize large-scale fabrication of ultrathin pure Li metal electrode by regular mechanical rolling operation.Free-standing ultrathin metallic Li foil cannot sustain operation for battery fabrication and large current in real application condition, it is of great importance for the employment of current collector with high conductivity and mechanical durability for the practical implantation of ultrathin metallic Li anode in high-energy-density batteries, which is similar to metal current collector for traditional porous electrodes (e.g., graphite on Cu foil). Cu foil is lithiophobic to molten lithium, which

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Section: Introductionmentioning

confidence: 99%

Doctor‐Blade Casting Fabrication of Ultrathin Li Metal Electrode for High‐Energy‐Density Batteries

Wang

Wan

et al. 2021

Advanced Energy Materials

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“…As one of the main challenges to the commercialization of SSBs, it is essential to consider the types of interphases formed at the electrode–electrolyte boundary 50,84,85 . A thermodynamically stable interface is desired, where the SSE does not react with the electrode, and a well‐defined interface is formed, but in most cases, thermodynamically unstable interphases are formed due to the interdiffusion of elements from both sides of the electrode SSE 86 . Furthermore, the conductive properties of the interphase can have a substantial effect on the performance of the cell (e.g., ionic and electronic conductivities).…”

Section: In Situ Surface‐sensitive X‐ray Spectroscopy To Study Composition and Electronic Structural Changesmentioning

confidence: 99%

“…Furthermore, the conductive properties of the interphase can have a substantial effect on the performance of the cell (e.g., ionic and electronic conductivities). If the interphase has high ionic and electronic conductivities, it will continue to grow into the bulk of the materials as there is sufficient access to electrons 86–88 . However, a kinetically stabilized interphase can be formed if it has negligible electronic conductivity but high lithium conductivity.…”

Section: In Situ Surface‐sensitive X‐ray Spectroscopy To Study Composition and Electronic Structural Changesmentioning

confidence: 99%

In situ characterizations of solid–solid interfaces in solid‐state batteries using synchrotron X‐ray techniques

2021

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The solid–solid electrode–electrolyte interface represents an important component in solid‐state batteries (SSBs), as ionic diffusion, reaction, transformation, and restructuring could all take place. As these processes strongly influence the battery performance, studying the evolution of the solid–solid interfaces, particularly in situ during battery operation, can provide insights to establish the structure–property relationship for SSBs. Synchrotron X‐ray techniques, owing to their unique penetration power and diverse approaches, are suitable to investigate the buried interfaces and examine structural, compositional, and morphological changes. In this review, we will discuss various surface‐sensitive synchrotron‐based scattering, spectroscopy, and imaging methods for the in situ characterization of solid–solid interfaces and how this information can be correlated to the electrochemical properties of SSBs. The goal is to overview the advantages and disadvantages of each technique by highlighting representative examples, so that similar strategies can be applied by battery researchers and beyond to study similar solid‐solid interface systems.

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“…[ 25 ] Despite these promising performances, the atomistic mechanism of Li and Na deposition and the reasons behind high CE and non‐dendritic plating have not been well understood. Thermodynamically controlled interfacial engineering may eliminate dendrites formation, [ 26 ] but its realization requires understanding of Li nucleation and growth mechanisms. Herein, the deposition mechanism of Li on Ti 3 C 2 T x was comprehensively studied at the atomistic scale by ab initio calculations.…”

Section: Introductionmentioning

confidence: 99%

Mechanisms of the Planar Growth of Lithium Metal Enabled by the 2D Lattice Confinement from a Ti₃C₂T_x MXene Intermediate Layer

Yang

Zhao

Lian

et al. 2021

Adv Funct Materials

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The propensity of Li to form irregular and nonplanar electrodeposits has become a fundamental barrier for fabricating Li metal batteries. Here, a planar, dendrite‐free Li metal growth on 2D Ti3C2Tx MXene is reported. Ab initio calculations suggest that Li forms a hexagonal close‐packed (hcp) layer on the surface of Ti3C2Tx via ionic bonding and the lattice confinement. The ionic bonding weakens gradually after a few monolayers, resulting in a nanometers‐thin transition region of hcp‐Li. Above this transition region, the deposition is dominated by plating of body‐centered cubic (bcc) Li via metallic bonding. Formation of a dense and planar Li metal anode with preferential growth along the (110) facet is explained by the lattice matching between Ti3C2Tx and hcp‐Li and then with bcc‐Li, as well as preferred thermodynamic factors including the large dendrite formation energy and small migration barrier for Li. The prepared Li metal anode shows stable cycling in a wide current density range from 0.5 to 10.0 mA cm–2. The LiFePO4‖Li full cell fabricated with this Li metal anode exhibits only 9.5% capacity fading after 500 charge–discharge cycles at 1 C rate.

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A Perspective on interfacial engineering of lithium metal anodes and beyond

Cited by 21 publications

References 108 publications

Doctor‐Blade Casting Fabrication of Ultrathin Li Metal Electrode for High‐Energy‐Density Batteries

Doctor‐Blade Casting Fabrication of Ultrathin Li Metal Electrode for High‐Energy‐Density Batteries

In situ characterizations of solid–solid interfaces in solid‐state batteries using synchrotron X‐ray techniques

Mechanisms of the Planar Growth of Lithium Metal Enabled by the 2D Lattice Confinement from a Ti₃C₂T_x MXene Intermediate Layer

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A Perspective on interfacial engineering of lithium metal anodes and beyond

Cited by 21 publications

References 108 publications

Doctor‐Blade Casting Fabrication of Ultrathin Li Metal Electrode for High‐Energy‐Density Batteries

Doctor‐Blade Casting Fabrication of Ultrathin Li Metal Electrode for High‐Energy‐Density Batteries

In situ characterizations of solid–solid interfaces in solid‐state batteries using synchrotron X‐ray techniques

Mechanisms of the Planar Growth of Lithium Metal Enabled by the 2D Lattice Confinement from a Ti3C2Tx MXene Intermediate Layer

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Product

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Mechanisms of the Planar Growth of Lithium Metal Enabled by the 2D Lattice Confinement from a Ti₃C₂T_x MXene Intermediate Layer