A Metal–Organic‐Framework‐Based Electrolyte with Nanowetted Interfaces for High‐Energy‐Density Solid‐State Lithium Battery

Abstract

Solid-state batteries (SSBs) are promising for safer energy storage, but their active loading and energy density have been limited by large interfacial impedance caused by the poor Li transport kinetics between the solid-state electrolyte and the electrode materials. To address the interfacial issue and achieve higher energy density, herein, a novel solid-like electrolyte (SLE) based on ionic-liquid-impregnated metal-organic framework nanocrystals (Li-IL@MOF) is reported, which demonstrates excellent electrochemical properties, including a high room-temperature ionic conductivity of 3.0 × 10 S cm , an improved Li transference number of 0.36, and good compatibilities against both Li metal and active electrodes with low interfacial resistances. The Li-IL@MOF SLE is further integrated into a rechargeable Li|LiFePO SSB with an unprecedented active loading of 25 mg cm , and the battery exhibits remarkable performance over a wide temperature range from -20 up to 150 °C. Besides the intrinsically high ionic conductivity of Li-IL@MOF, the unique interfacial contact between the SLE and the active electrodes owing to an interfacial wettability effect of the nanoconfined Li-IL guests, which creates an effective 3D Li conductive network throughout the whole battery, is considered to be the key factor for the excellent performance of the SSB.

Nanostructured Metal–Organic Framework (MOF)‐Derived Solid Electrolytes Realizing Fast Lithium Ion Transportation Kinetics in Solid‐State Batteries

“…The lithium ion transference number calculated from the DC polarization curve in Figure c is 0.33, which is higher than that of Li‐IL; such a phenomenon could be ascribed to the confinement effect of the Uio‐66 nanopores to [EMIM] + and [TFSI] − ions of large sizes.…”

Recent Progress of Hybrid Solid‐State Electrolytes for Lithium Batteries

“…[62] It presentsahigh room temperature ionic conductivity of 3.0 10 À4 Scm À1 and improved Li + transference number of 0.36, attributing to aw ell-connected 3D Li + conductive network and nanowetted interface between electrolyte and electrodes. [62] It presentsahigh room temperature ionic conductivity of 3.0 10 À4 Scm À1 and improved Li + transference number of 0.36, attributing to aw ell-connected 3D Li + conductive network and nanowetted interface between electrolyte and electrodes.…”

Bottom‐Up Fabrication of 1D Cu‐based Conductive Metal–Organic Framework Nanowires as a High‐Rate Anode towards Efficient Lithium Storage

“…[1] Accordingly,M OFs have been utilized in versatile applicationsi ncluding electrically transduced chemical sensors, MOF-based electronics, energy conversion,a nd electrochemically controlled capture and release. [2] Nevertheless, their utilization in energy-related applications has been confined to use as precursors or templates for carbons and/ort ransitionmetal oxides( TMOs) and even their hybrids. [2] Nevertheless, their utilization in energy-related applications has been confined to use as precursors or templates for carbons and/ort ransitionmetal oxides( TMOs) and even their hybrids.…”