Lithium metal anodes have attracted extensive attention owing to their high theoretical specific capacity. However, the notorious reactivity of lithium prevents their practical applications, as evidenced by the undesired lithium dendrite growth and unstable solid electrolyte interphase formation. Here, we develop a facile, cost-effective and one-step approach to create an artificial lithium metal/electrolyte interphase by treating the lithium anode with a tin-containing electrolyte. As a result, an artificial solid electrolyte interphase composed of lithium fluoride, tin, and the tin-lithium alloy is formed, which not only ensures fast lithium-ion diffusion and suppresses lithium dendrite growth but also brings a synergistic effect of storing lithium via a reversible tin-lithium alloy formation and enabling lithium plating underneath it. With such an artificial solid electrolyte interphase, lithium symmetrical cells show outstanding plating/stripping cycles, and the full cell exhibits remarkably better cycling stability and capacity retention as well as capacity utilization at high rates compared to bare lithium. Here the authors report a simple method to create a solid electrolyte interphase that is tightly anchored onto the surface of lithium metal anode. This artificial structure suppresses dead and dendrite Li and stores Li via formation of alloys, enabling impressive battery performance.

/pdf/fluorinated-hybrid-solid-electrolyte-interphase-for-dendrite-4vg1vncli2.pdf

Fluorinated hybrid solid-electrolyte-interphase for dendrite-free lithium deposition.

Ionic liquids for high performance lithium metal batteries

A Review of Composite Lithium Metal Anode for Practical Applications

Nanostructured magnesium nickel oxide (Mg₀.₆Ni₀.₄O) was synthesized by a self-propagating high temperature synthesis method followed by heat treatment. The particles of the resulting oxide were used as additives to prepare the sulfur/polyacrylonitrile/Mg₀.₆Ni₀.₄O (S/PAN/Mg₀.₆Ni₀.₄O) composite via wet ballmilling. The SEM observation revealed that the composite morphology was drastically changed by the addition of Mg₀.₆Ni₀.₄O, from smooth bulky particles of S/PAN to rough nanostructured agglomerates with two times the increase in the specific surface area, favouring the reactivity of the composite, and a homogeneous component distribution. Cyclic voltammetry, discharge–charge tests and ac impedance spectroscopy have shown improved conductivity and electrochemical properties of the composite by the addition of Mg₀.₆Ni₀.₄O, leading to high sulfur utilization and interfacial stabilization in a Li/S cell upon discharge–charge cycling. The cell demonstrated enhanced reversibility, resulting in a discharge capacity of about 1223 mA h g⁻¹ at the second cycle and retained about 100% of this value over 100 cycles. Furthermore, the S/PAN/Mg₀.₆Ni₀.₄O composite cathode exhibited a good rate capability with discharge capacities of 887, 710 and 445 mA h g⁻¹ at 0.5, 0.7 and 1 C, respectively.

Ternary sulfur/polyacrylonitrile/Mg₀.₆Ni₀.₄O composite cathodes for high performance lithium/sulfur batteries

Lithium metal batteries (LMBs) are representative of post-lithium-ion batteries with the great promise of increasing the energy density drastically by utilizing the low operating voltage and high specific capacity of metallic lithium. LMBs currently stand at a point of transition at which the accumulation of knowledge from fundamental research is being translated into large-scale commercialization. This review summarizes the available strategies for addressing the intrinsic shortcomings of LMBs, such as the suppression of dendritic growth and parasitic reactions from the material to the electrode to the cell level. The discussion pertaining to the cell level includes efforts and concerns relating to scaling up established knowledge and expertise with the view of commercialization. This article intends to encourage researchers in both fundamental research institutions and industry to make a synergistic effort and share their views comprehensively to ensure that LMB technology continues to evolve in harmony to become a mature technology. This article is protected by copyright. All rights reserved.

Lithium Metal Batteries: From Fundamental Research to Industrialization.

Multifunctional roles of carbon‐based hosts for Li‐metal anodes: A review

Lithium (Li) metal is regarded as one of the most promising anode candidates for next-generation energy storage systems due to its high theoretical capacity and low operating voltage. However, the growth of lithium dendrites caused by inhomogeneous and uncontrolled Li deposition hinders its practical application. Herein, a 3D porous lithiophilic zinc (Zn) scaffold modified with a thin zinc oxide (ZnO) surface layer on Cu foil (Zn/ZnO/Cu) as a current collector for lithium metal anodes is constructed by magnetron sputtering. The Zn/ZnO scaffold would react with Li+ ions before the deposition of lithium metal, leading to the formation of a Li–Zn alloy scaffold with a Li2O modified layer (Li–Zn/Li2O) on its surface. The surface Li2O layer with high ionic conductivity would passivate the conductive surface and provide a potential gradient across the surface layer and 3D porous Li–Zn alloy scaffold. Consequently, a Zn/ZnO@Li|Li symmetric cell can cycle stably for more than 500 h at 4 mA cm−2 for a total capacity of 1 mA h cm−2 and a low polarization (around 40 mV). Moreover, an ultra-long cycling life with a high capacity retention of 81% after 1000 cycles for a Li4Ti5O12|Zn/ZnO@Li full cell is also realized, showing that the Li–Zn/Li2O porous scaffold on Cu foil has a great prospect as a 3D current collector for Li metal anodes in the future.

Electrochemically induced highly ion conductive porous scaffolds to stabilize lithium deposition for lithium metal anodes

Dendrite-Free Reverse Lithium Deposition Induced by Ion Rectification Layer toward Superior Lithium Metal Batteries

Li metal anodes are undergoing a renaissance due to their ultra-high specific capacity and the lowest reduction potential. However, the practical application of Li-metal anodes is still challenged by Li dendrite growth and low coulombic efficiency (CE). Herein, a gradient Si-modified carbon paper (GSCP) made via magnetic sputtering is proposed to address these issues, in which the content of lithiophilic Si gradually decreases from the bottom to the top of the 3D host. Such a gradient lithiophilic structure can cause the Li metal to selectively nucleate and grow at the bottom first and then to the top part of GSCP, realizing stable Li plating/stripping and high space utilization of the 3D host simultaneously. Therefore, the designed GSCP composite anode achieves average CEs of 99.0% (400 cycles) and 97.0% (150 cycles) at 1 and 5 mA cm−2, respectively, and a prolonged lifespan (1350 h) with a low overpotential (∼15 mV). Remarkably, the GSCP@Li‖Li4Ti5O12 full cell exhibits high capacity retention of 84.5% after 5000 cycles at a 10C rate.

Bottom-top channeling Li nucleation and growth by a gradient lithiophilic 3D conductive host for highly stable Li-metal anodes

Promising Electrode and Electrolyte Materials for High-Energy-Density Thin-Film Lithium Batteries

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