Directed and Continuous Interfacial Channels for Optimized Ion Transport in Solid‐State Electrolytes

Abstract

The traditional strategy of using polymer solid electrolyte composite fillers is extremely limited by the continuity of the organic‐inorganic interface. Herein, a new composite electrolyte is fabricated, wherein alternating layers of organic polyethylene oxide (PEO) and inorganic molybdenum trioxide (MoO3) nanobelts are prepared and then the multilayer film is rolled and sliced into disks. Compared with a similar electrolyte prepared by disordered blending, the electrolyte here has a mesoscopic continuous organic‐inorganic interface perpendicular to the electrode direction. The ionic conductivity increases from 4.88 × 10−4 to 1.16 × 10−3 S cm−1. The “interfacial battery” can operate stably over >2000 charge–discharge cycles at 2 C (60 °C), and can withstand rapid charging–discharging, even at 10 C. Theoretical calculation results show that this unique assembly method essentially eliminates the energy band gap between the PEO and MoO3 interface, and promotes lithium ion (Li+) transport. In addition, the electronic interaction between the orbital of Mo and PEO extends the lattice structure of PEO, resulting in a reduction in the crystallinity, which further improves the battery performance. This study provides a composite electrolyte design that is different from blending and represents a new strategy for the development of low‐cost superionic conductors.

Reactive Aramid Nanofiber-Reinforced Polyvinyl-Alcohol-Based Solid Polymer Electrolyte for High-Performance Li Metal Batteries

“…The voltage of intercalation/deintercalation of LFP was performed at the reduction peak at 3.29 V and the oxidation peak at 3.59 V, separately. After the first cycle, the oxidation peak slightly shifted to 3.57 V while the reduction peak shifted to 3.28 V. The peak shifts are attributed to the amide group in the RANFs binding part of Li + in the first cycle . In the second and third cycles, the oxidation peaks and reduction peaks almost coincident, indicating that the electrolyte has excellent electrochemical stability and well capacity reversibility .…”

Squaraine-linked zwitterionic COF modified LLZTO nanoparticles for high performance polymer composite electrolytes in Li–S batteries

“…The modified porous polymer surface can effectively improve the electrode–electrolyte interface stability. 76,77…”

“…The modified porous polymer surface can effectively improve the electrode-electrolyte interface stability. 76,77 In situ Raman analysis was further applied to demonstrate the potential dependent evolution of sulfur speciation. The Raman spectra of LLZTO, HUT4 and PEO are shown in Fig.…”

Cellulose-Assisted Vertically Heterostructured PEO-Based Solid Electrolytes Mitigating Li-Succinonitrile Corrosion for Lithium Metal Batteries

“…Concerning the increased demands for energy storage and conversion devices, solid-state lithium metal batteries (SSLMBs) have been enthusiastically researched for their reliable safety, high capacity of the lithium (Li) anode, and enhanced battery energy density. − Based on the low cost, flexible preparation, and high compatibility with the Li anode, solid polymer electrolytes (SPEs) are one of the most promising candidates applied in SSLMBs. − Poly­(ethylene oxide) (PEO)-based SPEs have been pursued dramatically due to their advantages of high safety, high capacity, low cost, flexibility, excellent electrochemical performance, and good compatibility with lithium salts compared with other SPEs . Nevertheless, the application of PEO-based SPEs is still hindered by their low ionic conductivities and the narrow electrochemical stability window (ESW). , To address these problems, considerable strategies have been proposed, including the addition of functional materials and the design of unique electrolyte structures, such as roll-to-roll structures and vertical heterostructures. − …”