Aluminum Corrosion Chemistry in High-Voltage Lithium Metal Batteries with LiFSI-Based Ether Electrolytes.

High-voltage Li metal batteries (LMBs) based on ether electrolytes hold potential for achieving high energy densities exceeding 500 Wh kg, but face challenges with electrolyte oxidative stability, particularly concerning aluminum (Al) current collector corrosion. However, the specific chemistry behind Al corrosion and its effect on electrolyte components remains unexplored. Here, our study delves into Al corrosion in the representative LiFSI-DME electrolyte system, revealing that low-concentration electrolytes exacerbate Al current collector corrosion and solvent decomposition.

Fast Interfacial Defluorination Kinetics Enables Stable Cycling of Low-Temperature Lithium Metal Batteries.

The development of low-temperature lithium metal batteries (LMBs) encounters significant challenges because of severe dendritic lithium growth during the charging/discharging processes. To date, the precise origin of lithium dendrite formation still remains elusive due to the intricate interplay between the highly reactive lithium metal anode and organic electrolytes. Herein, we unveil the critical role of interfacial defluorination kinetics of localized high-concentration electrolytes (LHCEs) in regulating lithium dendrite formation, thereby determining the performance of low-temperature LMBs.

Amorphous Chloride Solid Electrolytes with High Li-Ion Conductivity for Stable Cycling of All-Solid-State High-Nickel Cathodes.

Solid electrolytes (SEs) are central components that enable high-performance, all-solid-state lithium batteries (ASSLBs). Amorphous SEs hold great potential for ASSLBs because their grain-boundary-free characteristics facilitate intact solid-solid contact and uniform Li-ion conduction for high-performance cathodes. However, amorphous oxide SEs with limited ionic conductivities and glassy sulfide SEs with narrow electrochemical windows cannot sustain high-nickel cathodes.

Origin of dendrite-free lithium deposition in concentrated electrolytes.

The electrolyte solvation structure and the solid-electrolyte interphase (SEI) formation are critical to dictate the morphology of lithium deposition in organic electrolytes. However, the link between the electrolyte solvation structure and SEI composition and its implications on lithium morphology evolution are poorly understood. Herein, we use a single-salt and single-solvent model electrolyte system to systematically study the correlation between the electrolyte solvation structure, SEI formation process and lithium deposition morphology.

Constructing Three-Dimensional Topological Zn Deposition for Long-Life Aqueous Zn-Ion Batteries.

Uniform and compact Zn deposition-dissolution is essential to achieve high Coulombic efficiency and long lifespan for Zn anodes. More attention has been commonly focused on the suppression of macroscopic Zn dendrites in the previous reports. The rational control of the microstructure of Zn deposition to prevent the intrinsic volume expansion and pulverization of Zn metal so as to stabilize Zn anodes is less discussed.

Rational Design of an Artificial SEI: Alloy/Solid Electrolyte Hybrid Layer for a Highly Reversible Na and K Metal Anode.

The practical application of a Na/K-metallic anode is intrinsically hindered by the poor cycle life and safety issues due to the unstable electrode/electrolyte interface and uncontrolled dendrite growth during cycling. Herein, we solve these issues through an reaction of an oxyhalogenide (BiOCl) and Na to construct an artificial solid electrolyte interphase (SEI) layer consisting of an alloy (NaBi) and a solid electrolyte (NaOCl) on the surface of the Na anode. As demonstrated by theoretical and experimental results, such an artificial SEI layer combines the synergistic properties of high ionic conductivity, electronic insulation, and interfacial stability, leading to uniform dendrite-free Na deposition beneath the hybrid SEI layer.

Revisiting the Role of Physical Confinement and Chemical Regulation of 3D Hosts for Dendrite-Free Li Metal Anode.

Lithium metal anode has been demonstrated as the most promising anode for lithium batteries because of its high theoretical capacity, but infinite volume change and dendritic growth during Li electrodeposition have prevented its practical applications. Both physical morphology confinement and chemical adsorption/diffusion regulation are two crucial approaches to designing lithiophilic materials to alleviate dendrite of Li metal anode. However, their roles in suppressing dendrite growth for long-life Li anode are not fully understood yet.

Surface Transformation Enables a Dendrite-Free Zinc-Metal Anode in Nonaqueous Electrolyte.

Significant challenges remain in developing rechargeable zinc batteries mainly because of reversibility problems on zinc-metal anodes. The dendritic growth and hydrogen evolution on zinc electrodes are major obstacles to overcome in developing practical and safe zinc batteries. Here, a dendrite-free and hydrogen-free Zn-metal anode with high Coulombic efficiency up to 99.

Artificial Heterogeneous Interphase Layer with Boosted Ion Affinity and Diffusion for Na/K-Metal Batteries.

Metallic Na (K) are considered a promising anode materials for Na-metal and K-metal batteries because of their high theoretical capacity, low electrode potential, and abundant resources. However, the uncontrolled growth of Na (K) dendrites severely damages the stability of the electrode/electrolyte interface, resulting in battery failure. Herein, a heterogeneous interface layer consisting of metal vanadium nanoparticles and sodium sulfide (potassium sulfide) is introduced on the surface of a Na (K) foil (i.

Regulating LiS Deposition by Ostwald Ripening in Lithium-Sulfur Batteries.

The lithium-sulfur (Li-S) batteries have attracted tremendous attention from both academia and industry for their high energy density and environmental benignity. However, the cell performance suffers from the passivation of the conductive matrix caused by uncontrolled lithium sulfide (LiS) deposition. Therefore, regulation of LiS deposition is essential to advanced Li-S batteries.

Design Principles of Sodium/Potassium Protection Layer for High-Power High-Energy Sodium/Potassium-Metal Batteries in Carbonate Electrolytes: a Case Study of Na Te/K Te.

The sodium (potassium)-metal anodes combine low-cost, high theoretical capacity, and high energy density, demonstrating promising application in sodium (potassium)-metal batteries. However, the dendrites' growth on the surface of Na (K) has impeded their practical application. Herein, density functional theory (DFT) results predict Na Te/K Te is beneficial for Na /K transport and can effectively suppress the formation of the dendrites because of low Na /K migration energy barrier and ultrahigh Na /K diffusion coefficient of 3.

Electrolyte Solvation Manipulation Enables Unprecedented Room-Temperature Calcium-Metal Batteries.

Calcium-metal batteries (CMBs) provide a promising option for high-energy and cost-effective energy-storage technology beyond the current state-of-the-art lithium-ion batteries. Nevertheless, the development of room-temperature CMBs is significantly impeded by the poor reversibility and short lifespan of the calcium-metal anode. A solvation manipulation strategy is reported to improve the plating/stripping reversibility of calcium-metal anodes by enhancing the desolvation kinetics of calcium ions in the electrolyte.

Enabling High-Voltage Lithium Metal Batteries by Manipulating Solvation Structure in Ester Electrolyte.

Lithium metal is an ideal electrode material for future rechargeable lithium metal batteries. However, the widespread deployment of metallic lithium anode is significantly hindered by its dendritic growth and low Coulombic efficiency, especially in ester solvents. Herein, by rationally manipulating the electrolyte solvation structure with a high donor number solvent, enhancement of the solubility of lithium nitrate in an ester-based electrolyte is successfully demonstrated, which enables high-voltage lithium metal batteries.

Stable cycling of Na metal anodes in a carbonate electrolyte.

It is significantly challenging to stabilize sodium metal anodes in carbonate electrolytes. Here, we report that a sodium metal anode can achieve a high coulombic efficiency of up to ∼97% over 400 cycles at 0.1 mA cm-2 in a carbonate electrolyte with NaAsF6 as an additive.