Lan Zhang

Using no solvents, dry processing technique (DPT), especially for binder fibrillation is drawing more research attention due to its feasibility in fabricating thick electrodes as well as ultra‐thin solid electrolyte (SE) films. However, DPT electrodes and SE films are still facing multiple challenges including processing sensitivity (to temperature, humidity, as well as particle size and mechanical properties of the electrode/electrolyte materials, to name but a few), poor compatibility with lithium metal anode, as well as hindered ion transportation, which are restricting their commercial applications. Focus on the charge percolating of the high loading DPT electrodes/SE films and their stability toward metal Li, the mainstream commercial electrode characteristics including area loading and porosity are begun with, then the latest advances on DPT is reviewed from the electrode and SE aspect, respectively. It is found that although DPT achieved great success in academic study, there's still a large space to be explored before it can energize the battery industry.

Anode‐free lithium metal batteries (AFLMBs) are attracting significant attention due to their easy fabrication and high volumetric energy density. However, inhomogeneous deposition of lithium usually leads to dead Li or dendrites, in the meantime, the limited active lithium inventory also restricts the cycle life of AFLMB. In this study, a mixed ion/electron conductive interlayer (SNAF) composed of Si nanoparticles, carbon nanotubes (CNT), lithium polyacrylic acid (PAALi), and LiF is designed to stabilize the deposition process of lithium. Of which Si serves as a lipophilic site and reduces the nuclei overpotential, CNT decreases the local current density and thus enhances the high current deposition stability, while PAALi and LiF work as an artificial solid electrolyte interphase (ASEI) and reduce the irreversible active Li loss. It shows that with SNAF interlayer, the thickness of the lithium deposition is close to the theoretical value even up to 10 mAh cm ⁻² , so as to the stripping process. Moreover, it also enabled the AFLMB to work even under the high current density of 4.29 mA cm ⁻² . It is believed this facile interlayer strategy can greatly promote the advancement of AFLMB research.

Thin and flexible solid‐state electrolyte (SSE) films with high ionic conductivity and low interfacial resistance are urgently required for lithium metal batteries (LMBs). However, it's still challenging to reduce the film thickness to 3 Zr ₂ Si ₂ PO ₁₂ (LZSP) films with ceramic content up to 91% using a composite polymer binder, polyvinylidene fluoride (PVDF), and polyethylene oxide (PEO). It shows that PEO not only enhanced the film flexibility but also makes it be easily peeled off to form a freestanding membrane, PLN. To promote the interfacial ion transport, PEO/lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) is introduced to the film surface, and the resultant tri‐layer film, PPLN, shows a satisfying room temperature ionic conductivity of 0.116 mS cm ⁻¹ , high Li ⁺ transference number of 0.79, and good compatibility with metal lithium. As a result, LMBs using LiFePO ₄ cathode and PPLN electrolyte exhibit excellent safety as well as electrochemical performances in the wide temperature range between room temperature (RT) and 100 °C.

A cathode with an areal capacity of more than 5 mA h cm ⁻² is crucial for practical Li–S batteries. Besides, reducing the electrolyte weight ratio, in both liquid and solid-state Li–S batteries, is also important.