A dielectric electrolyte composite with high lithium-ion conductivity for high-voltage solid-state lithium metal 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

From scientific and technological points of view, poly(vinylidene fluoride), PVDF, is one of the most exciting polymers due to its overall physicochemical characteristics. This polymer can crystalize into five crystalline phases and can be processed in the form of films, fibers, membranes, and specific microstructures, being the physical properties controllable over a wide range through appropriate chemical modifications. Moreover, PVDF-based materials are characterized by excellent chemical, mechanical, thermal, and radiation resistance, and for their outstanding electroactive properties, including high dielectric, piezoelectric, pyroelectric, and ferroelectric response, being the best among polymer systems and thus noteworthy for an increasing number of technologies. This review summarizes and critically discusses the latest advances in PVDF and its copolymers, composites, and blends, including their main characteristics and processability, together with their tailorability and implementation in areas including sensors, actuators, energy harvesting and storage devices, environmental membranes, microfluidic, tissue engineering, and antimicrobial applications. The main conclusions, challenges and future trends concerning materials and application areas are also presented.

pdf/smart-and-multifunctional-materials-based-on-electroactive-vf2wrky5so.pdf

Smart and Multifunctional Materials Based on Electroactive Poly(vinylidene fluoride): Recent Advances and Opportunities in Sensors, Actuators, Energy, Environmental, and Biomedical Applications.

Solid polymer electrolytes (SPEs) hold a great promise in the application of solid‐state lithium batteries, but suffer from poor mechanical properties and uncontrolled electrode/electrolyte interfacial reaction, which restrict their overall electrochemical performance. Herein, the design of 2D fluorinated graphene‐reinforced PVDF‐HFP‐LiTFSI (FPH‐Li) polymer electrolytes to address these challenges is reported. Uniformly dispersed fluorinated graphene induces a unique grain refinement effect, which effectively improves the mechanical properties without excessively increasing the thickness of the polymer electrolyte. Significant reduction in polymer grain size enhances interfacial lithium ion (Li‐ion) transport and homogenizes Li‐ion flux, thereby improving Li‐ion conductivity and promoting uniform Li plating/stripping. Furthermore, extensive characterizations show that fluorinated graphene is involved in the construction of a stable artificial interface, which effectively prevents the side reactions between the lithium metal anode and solvated molecules. As a result, the use of thin FPH‐Li polymer electrolytes (thickness of ≈45 µm) enables long‐term Li plating/stripping with a small overpotential in Li/Li symmetrical cells and stable cycling of Li/LiNi0.6Co0.2Mn0.2O2 full cells with a high average Coulombic efficiency of 99.5% at 1.0 C. This work verifies the effectiveness of 2D materials in improving the comprehensive properties of polymer electrolytes and promotes the applications of SPEs in high‐performance solid‐state lithium batteries.

Two‐Dimensional Fluorinated Graphene Reinforced Solid Polymer Electrolytes for High‐Performance Solid‐State Lithium Batteries

Solid polymer electrolytes with large ionic conductivity, high ionic transference number, and good interfacial compatibility with electrodes are highly desired for solid‐state batteries. However, unwanted polarizations and side reactions occurring in traditional dual‐ion polymer conductors hinder their practical applications. Here, single‐ion polymer conductors (SIPCs) with exceptional selectivity for Li‐ion conduction (Li‐ion transference number up to 0.93), high room‐temperature ionic conductivity of about 10−4 S cm−1, and a wide electrochemical stability window (>4.5 V, vs Li/Li+) are prepared by precisely regulating the ion–dipole interactions between Li+ and carbonyl/cyano groups. The resulting SIPCs show an excellent electrochemical stability with Li metal during long‐term cycling at room temperature and 60 °C. LiFePO4‐based solid‐state cells containing the SIPCs exhibit good rate and cycling performance in a wide temperature range from −20 to 90 °C. By the same way of ion–dipole interaction regulation, sodium‐ and potassium‐based SIPCs with both high ionic conductivity and high cationic transference numbers are also prepared. The findings in this work provide guidance for the development of high‐performance SIPCs and other metal‐ion systems beyond Li+.

Ion–Dipole Interaction Regulation Enables High‐Performance Single‐Ion Polymer Conductors for Solid‐State Batteries

The extremely low room-temperature ionic conductivity of solid-state polymer electrolytes (SPEs) ranging from 10−7 to 10−5 S cm−1 seriously restricts their practical application in solid-state lithium metal batteries (LMBs). Herein, a unique relaxor ferroelectric (RFE) polymer of poly(vinylidene fluoride-co-trifluoroethylene-co-chlorotrifluoroethylene) [P(VDF-TrFE-CTFE)] is first investigated as a matrix of SPEs. We find that the P(VDF-TrFE-CTFE) with an ultrahigh dielectric constant (er) of 44 presents a stronger solvation ability towards lithium ions, which promotes the dissociation of LiN(SO2CF3)2 to form more free charge carriers and enhances their mobility compared to the conventional PVDF with a low er of 9. The P(VDF-TrFE-CTFE) based SPEs show a much higher ionic conductivity of 3.10 × 10−4 S cm−1 at 25 °C and lower activation energy (0.26 eV) than PVDF based SPEs (1.77 × 10−5 S cm−1 and 0.49 eV). The PVDF blended with the P(VDF-TrFE-CTFE) or dielectric fillers such as BaTiO3 further confirm that the hybrid electrolytes with a larger er show a higher ionic conductivity. In addition, very tight interfaces of P(VDF-TrFE-CTFE) based SPEs with both the cathode and Li metal anode are constructed to ensure a stable interfacial resistance during cycling. The LiFePO4/Li and LiNi0.8Co0.1Mo0.1O2/Li batteries using P(VDF-TrFE-CTFE) based SPEs present a stable cycling performance at 25 °C. This work proposes a new strategy and opens a new research area to construct SPEs with high ionic conductivity by greatly increasing the er of polymers.

A relaxor ferroelectric polymer with an ultrahigh dielectric constant largely promotes the dissociation of lithium salts to achieve high ionic conductivity

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A relaxor ferroelectric polymer with an ultrahigh dielectric constant largely promotes the dissociation of lithium salts to achieve high ionic conductivity