The immerging three dimensional (3D) metal-organic framework (MOF)-reinforced composite solid-state electrolytes have attracted great interest because of the enhanced ionic conductivity and mechanical properties. However, the defective spatial arrangement of MOFs restricted by fabrication methodology leads to insufficient lithium ion transport in electrolytes. Herein, a 3D interconnected MOF framework tailored for all-solid-state electrolytes is rationally designed by a universal polydopamine (PDA)-engineered “double-sided tape” strategy. The PDA serves as a double-sided tape, firmly adhering on the special single-layer Nylon grid as well as offering uniform nucleation sites to anchor the metal nodes to ensure continuous growth of well-ordered MOFs. Benefiting from the Lewis acid feature of MOFs and its cage effect toward TFSI−, a fast and homogeneous lithium ion transport can be achieved through the internal channels within neighboring MOFs and the continuous MOFs/polymer interfaces both along the short-range circumferential boundary of Nylon fiber. The resultant composite electrolytes exhibit high lithium ion conductivity and prominent mechanical properties, rendering excellent cyclic stability whether used in coin or pouch cells. This work demonstrates a widely applicable “double-sided tape” strategy for controllable spatial arrangement of MOF nanoparticles on optional substrates, which provides a scalable approach to rationally construct desired lithium ion pathways within composite electrolytes.

Polypropylene separator-reinforced polymer-in-salt SSCEs combine high ionic conductivity, largetLi+and superior interface stability toward lithium anodes, enabling excellent cycling stability of solid-state lithium ion batteries at room temperature.

A solid composite electrolyte-like bifunctional separator customized for lithium metal batteries, is developed by wrapping a PP substrate with PVDF–DBDPO layers on both sides, enabling high fire resistance and excellent cycling performance.

Solid-state polymer electrolytes (SSPEs) for room-temperature lithium ion batteries (LIBs) usually suffer from the uncontrollable lithium dendrite propagation due to the mechanical weakness. Herein, through a facile double-side coating strategy, novel sandwich-like poly (vinylidene fluoride) (PVDF)-based electrolyte membranes that are mechanically reinforced by polypropylene (PP) separator are successfully developed for high-performance room-temperature solid-state LIBs. With a small amount of bound dimethylformamide (DMF) to serve as a plasticizer for the PVDF polymer host, the as-prepared PVDF/PP SSPEs achieve a high ionic conductivity of 1.53 x 10(-4) S cm(-1). The robust commercial PP separator can significantly improve the mechanical properties of the sandwich SSPEs, and more importantly it functions as physical obstacle here to restrain lithium dendrite growth during the repeated charge-discharge cycling. The solid-state batteries assembled with the PVDF/PP SSPEs, LiFePO4 (LFP) cathode and lithium anode thus exhibit dramatically enhanced cycling performance compared with the batteries based on blank PVDF SSPEs, delivering a high specific capacitance of 134 mAh g(-1) and 97% capacity retention over 180 cycles under 0.3C at room temperature. Such high-performance PVDF/PP SSPEs with the facile and scalable fabrication, together with the low-cost and widely available raw materials, are highly promising electrolytes for room-temperature solid-state LIBs.