DataSheet1_Metal-organic framework (MOF)-incorporated polymeric electrolyte realizing fast lithium-ion transportation with high Li+ transference number for solid-state batteries.docx

Composite polymer electrolytes (CPEs) show significant advantages in developing solid-state batteries due to their high flexibility and easy processability. In CPEs, solid fillers play a considerable effect on electrochemical performances. Recently, metal-organic frameworks (MOFs) are emerging as new solid fillers and show great promise to regulate ion migration. Herein, by using a Co-based MOF, a high-performance CPE is initially prepared and studied. Benefiting from the sufficient interactions and pore confinement from MOF, the obtained CPE shows both high ionic conductivity and a high Li+ transference number (0.41). The MOF-incorporated CPE then enables a uniform Li deposition and stable interfacial condition. Accordingly, the as-assembled solid batteries demonstrate a high reversible capacity and good cycling performance. This work verifies the practicability of MOFs as solid fillers to produce advanced CPEs, presenting their promising prospect for practical application.</p

Antiperovskite Electrolytes for Solid-State Batteries

Solid-state batteries have fascinated the research community over the past decade, largely due to their improved safety properties and potential for high-energy density. Searching for fast ion conductors with sufficient electrochemical and chemical stabilities is at the heart of solid-state battery research and applications. Recently, significant progress has been made in solid-state electrolyte development. Sulfide-, oxide-, and halide-based electrolytes have been able to achieve high ionic conductivities of more than 10–3 S/cm at room temperature, which are comparable to liquid-based electrolytes. However, their stability toward Li metal anodes poses significant challenges for these electrolytes. The existence of non-Li cations that can be reduced by Li metal in these electrolytes hinders the application of Li anode and therefore poses an obstacle toward achieving high-energy density. The finding of antiperovskites as ionic conductors in recent years has demonstrated a new and exciting solution. These materials, mainly constructed from Li (or Na), O, and Cl (or Br), are lightweight and electrochemically stable toward metallic Li and possess promising ionic conductivity. Because of the structural flexibility and tunability, antiperovskite electrolytes are excellent candidates for solid-state battery applications, and researchers are still exploring the relationship between their structure and ion diffusion behavior. Herein, the recent progress of antiperovskites for solid-state batteries is reviewed, and the strategies to tune the ionic conductivity by structural manipulation are summarized. Major challenges and future directions are discussed to facilitate the development of antiperovskite-based solid-state batteries

Nanostructured Electrode Materials Derived from Metal–Organic Framework Xerogels for High-Energy-Density Asymmetric Supercapacitor

This work successfully demonstrates metal–organic framework (MOF) derived strategy to prepare nanoporous carbon (NPC) with or without Fe₃O₄/Fe nanoparticles by the optimization of calcination temperature as highly active electrode materials for asymmetric supercapacitors (ASC). The nanostructured Fe₃O₄/Fe/C hybrid shows high specific capacitance of 600 F/g at a current density of 1 A/g and excellent capacitance retention up to 500 F/g at 8 A/g. Furthermore, hierarchically NPC with high surface area also obtained from MOF gels displays excellent electrochemical performance of 272 F/g at 2 mV/s. Considering practical applications, aqueous ASC (aASC) was also assembled, which shows high energy density of 17.496 Wh/kg at the power density of 388.8 W/kg. The high energy density and excellent capacity retention of the developed materials show great promise for the practical utilization of these energy storage devices

Stabilization of NASICON-Type Electrolyte against Li Anode via an Ionic Conductive MOF-Incorporated Adhesive Interlayer

Sodium superionic conductor (NASICON)-type electrolytes with high ionic conductivity and moisture/air stability are essential for solid-state batteries. However, they generally suffer from poor electrochemical stability and insufficient contact against Li metal, causing severe performance degradation. To address this challenge, an ionic conductive metal–organic framework (MOF)-incorporated polymeric layer (denoted as ZCPL) is prepared and used as the coating layer of Li1.5Al0.5Ge1.5(PO4)3 (LAGP). As a protective layer, ZCPL can effectively prevent the redox reaciton between LAGP and Li metal, eliminating the formation of detrimental interphases and cracks upon battery cycling. The adhesive ZCPL can also infiltrate into the void/gaps of the LAGP surface, generating a firm connection with intimate contact. Besides, ZCPL with good ionic conductivity and a soft texture provides rich pathways for fast Li+ transport and ensures a uniform Li+ flow through the interface. Benefiting from ZCPL, both the Li symmerical cell and Li/LiFePO4 full cell show long-term cycling stability

Presentation1_Li-Rich Antiperovskite/Nitrile Butadiene Rubber Composite Electrolyte for Sheet-Type Solid-State Lithium Metal Battery.pdf

Lithium-rich antiperovskites (LiRAPs) hold great promise to be the choice of solid-state electrolytes (SSEs) owing to their high ionic conductivity, low activation energy, and low cost. However, processing sheet-type solid-state Li metal batteries (SSLiB) with LiRAPs remains challenging due to the lack of robust techniques for battery processing. Herein, we propose a scalable slurry-based procedure to prepare a flexible composite electrolyte (CPE), in which LiRAP (e.g., Li2OHCl0.5Br0.5, LOCB) and nitrile butadiene rubber (NBR) serve as an active filler and as a polymer scaffold, respectively. The low-polar solvent helps to stabilize the LiRAP phase during slurry processing. It is found that the addition of LOCB into the NBR polymer enhances the Li ion conductivity for 2.3 times at 60°C and reduces the activation energy (max. 0.07 eV). The as-prepared LOCB/NBR CPE film exhibits an improved critical current of 0.4 mA cm−2 and can stably cycle for over 1000 h at 0.04 mA cm−2 under 60°C. In the SSLiB with the sheet-type configuration of LiFePO4(LFP)||LOCB/NBR CPE||Li, LFP exhibits a capacity of 137 mAh/g under 60 at 0.1°C. This work delivers an effective strategy for fabrication of LiRAP-based CPE film, advancing the LiRAP-family SSEs toward practical applications.</p