Understanding and suppression strategies toward stable Li metal anode for safe lithium batteries

Solid-state electrolytes (SSEs) are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density. Among them, polymer solid-state electrolytes (PSEs) are competitive candidates for replacing commercial liquid electrolytes due to their flexibility, shape versatility and easy machinability. Despite the rapid development of PSEs, their practical application still faces obstacles including poor ionic conductivity, narrow electrochemical stable window and inferior mechanical strength. Polymer/inorganic composite electrolytes (PIEs) formed by adding ceramic fillers in PSEs merge the benefits of PSEs and inorganic solid-state electrolytes (ISEs), exhibiting appreciable comprehensive properties due to the abundant interfaces with unique characteristics. Some PIEs are highly compatible with high-voltage cathode and lithium metal anode, which offer desirable access to obtaining lithium metal batteries with high energy density. This review elucidates the current issues and recent advances in PIEs. The performance of PIEs was remarkably influenced by the characteristics of the fillers including type, content, morphology, arrangement and surface groups. We focus on the molecular interaction between different components in the composite environment for designing high-performance PIEs. Finally, the obstacles and opportunities for creating high-performance PIEs are outlined. This review aims to provide some theoretical guidance and direction for the development of PIEs. 

/pdf/tailoring-practically-accessible-polymer-inorganic-composite-2rlpdk5s.pdf

Tailoring Practically Accessible Polymer/Inorganic Composite Electrolytes for All-Solid-State Lithium Metal Batteries: A Review

Sulfide solid electrolytes (SEs) are recognized as one of the most promising candidates for all-solid-state batteries (ASSBs), due to their superior ionic conductivity and remarkable ductility. However, poor air stability, complex synthesis process, low yield, and high production cost obstruct the large-scale application of sulfide SEs. Herein, a one-step gas-phase synthesis method for sulfide SEs with oxide raw materials in ambient air, completely getting rid of the glovebox and thus making large-scale production possible, is reported. By adjusting substituted elements and concentrations, the ionic conductivity of Li4- x Sn1- x Mx S4 can reach 2.45 mS cm-1 , which represents the highest value among all reported moist-air-stable and recoverable lithium-ion sulfide SEs reported. Furthermore, ASSBs with air/water-exposed and moderate-temperature-treated Li3.875 Sn0.875 As0.125 S4 even maintains superior performances with the highest reversible capacity (188.4 mAh g-1 ) and the longest cycle life (210 cycles), which also breaks the record. Therefore, it may become one of the most critical breakthroughs during the development of sulfide ASSBs toward its practical application and commercialization.

Superior All-Solid-State Batteries Enabled by a Gas-Phase-Synthesized Sulfide Electrolyte with Ultrahigh Moisture Stability and Ionic Conductivity.

Magnesium-based batteries represent one of the successfully emerging electrochemical energy storage chemistries, mainly due to the high theoretical volumetric capacity of metallic magnesium (i.e., 3833 mAh cm−3 vs. 2046 mAh cm−3 for lithium), its low reduction potential (−2.37 V vs. SHE), abundance in the Earth’s crust (104 times higher than that of lithium) and dendrite-free behaviour when used as an anode during cycling. However, Mg deposition and dissolution processes in polar organic electrolytes lead to the formation of a passivation film bearing an insulating effect towards Mg2+ ions. Several strategies to overcome this drawback have been recently proposed, keeping as a main goal that of reducing the formation of such passivation layers and improving the magnesium-related kinetics. This manuscript offers a literature analysis on this topic, starting with a rapid overview on magnesium batteries as a feasible strategy for storing electricity coming from renewables, and then addressing the most relevant outcomes in the field of anodic materials (i.e., metallic magnesium, bismuth-, titanium- and tin-based electrodes, biphasic alloys, nanostructured metal oxides, boron clusters, graphene-based electrodes, etc.).

/pdf/an-overview-on-anodes-for-magnesium-batteries-challenges-pvf91rw2bf.pdf

An Overview on Anodes for Magnesium Batteries: Challenges towards a Promising Storage Solution for Renewables.

All‐solid‐state batteries (ASSBs) using sulfide electrolytes have attracted ever‐increasing interest due to high ionic conductivity of the sulfides. Nevertheless, a thin, strong solid‐state sulfide electrolyte membrane maintaining high ionic conductivity is highly desired for ASSBs. Here, a thin, flexible composite solid electrolyte membrane composed of argyrodite sulfide Li6PS5Cl and a polar poly(vinylidene fluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) framework is prepared via an electrospinning‐infiltration‐hot‐pressing method. The interaction between Li6PS5Cl and polar P(VDF‐TrFE) ensures a high lithium‐ion conductivity (≈1.2 mS cm–1) at room temperature and good mechanical ductility of the composite electrolyte membrane. The coin‐type ASSB cells with the thin composite electrolyte membrane, a composite cathode of LiNbO3‐coated LiNi0.8Co0.1Mn0.1O2 and Li6PS5Cl, and a lithium‐indium anode, show super cycling performance, and the capacity retention is 92% after 1000 cycles and 71% even after 20 000 cycles at 1.0 mA cm–2 (i.e., 1.61 C) at room temperature. Moreover, pouch‐type ASSB cells with a high mass loading of active materials are made to demonstrate the potential and feasibility in future commercial applications.

Super Long‐Cycling All‐Solid‐State Battery with Thin Li6PS5Cl‐Based Electrolyte

Covalent interfacial coupling for hybrid solid-state Li ion conductor

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Covalent interfacial coupling for hybrid solid-state Li ion conductor