Insights into the Enhanced Interfacial Stability Enabled by Electronic Conductor Layers in Solid‐State Li Batteries

Abstract

The (electro)chemical reactions between Li1.3Al0.3Ti1.7(PO4)3 (LATP) solid‐state electrolyte and lithium metal plague the practical applications of LATP. A commonly used strategy to tackle this issue is to construct an ionic conductor layer to stabilize Li/LATP interface. Herein, it is demonstrated that an electronic conductor interlayer (Al or Ag) can also greatly enhance the interfacial stability of Li/LATP. To unveil the origin of the enhanced interfacial stability, a series of techniques, including in situ electron and optical microscopies, kelvin probe force microscopy, and finite element analysis, is exploited. Control experiments show clearly that Al layer can effectively homogenize the electric field distribution, which enables the uniform growth of interphases and thus prevents stress concentration and crack propagation. Moreover, when coupled with solid polymer electrolyte (SPE) to form Al‐SPE bilayer, it can effectively protect LATP from electron attack and interphase formation. Remarkably, Li symmetrical cells with an Al‐SPE bilayer exhibit superior stability of more than 5000 h at 0.2 mA cm−2, among the best cycling performances to date. This work presents an in‐depth understanding of the mechanism of the enhanced interfacial stability enabled by electronic conductor interlayers, as well as a universal interface architecture to boost the cyclability of solid‐state batteries.

Synergistic Strategy Using Doping and Polymeric Coating Enables High-Performance High-Nickel Layered Cathodes for Lithium-Ion Batteries

“…Human energy consumption is rising annually as industrialization picks up speed, and the energy crisis has increasingly become the major obstacle restricting countries worldwide from achieving technological breakthroughs. − Due to the sustainability of energy transmission and distribution, electrical energy storage (EES) has gained recognition as a technology that can successfully address these challenges. Lithium-ion batteries (LIBs) are being developed increasingly in the direction of high-performance battery systems with high specific energy, high power density, high safety, and long cycle life as an emerging high-efficiency and clean energy storage device. − The cathode material, which is a crucial component of LIBs, is what primarily determines the electrochemical performance of LIBs, including energy density, cycling stability, and preparation cost.…”

Building better solid‐state batteries with silicon‐based anodes

“…In addition, it should be mentioned that, in practice, the cathode side, and some extra conductive agents, that is, SSEs, are necessary to obtain a satisfactory contact condition. [ 27 ]…”

“…In addition, it should be mentioned that, in practice, the cathode side, and some extra conductive agents, that is, SSEs, are necessary to obtain a satisfactory contact condition. [27] F I G U R E 4 Development roadmap of Si-based anodes in Si-SSBs as summarized based on the type of SSEs. Reproduced with permission.…”

“…[21][22][23][24][25] Accordingly, various strategies have been designed to solve the Li dendrite growth and interfacial issues in LMSSBs, such as the surface modification of Li metal anodes, the imposed external stack pressure for ensuring interfacial contact, and the structural and composition optimization for SSEs and Li metal anodes. [26][27][28][29][30] The development of LMSSBs can be facilitated by such beneficial explorations, but the commercialization of LMSSBs remains a significant challenge. In this regard, greater attention has to be paid to investigating solid-state batteries (SSBs) along with other high-capacity anodes, especially alloy anodes.…”

Multi‐Physical Field Simulation: A Powerful Tool for Accelerating Exploration of High‐Energy‐Density Rechargeable Lithium Batteries

“…[ 72,75 ] Based on the successful practices, MPF simulation has been employed to uncover the underlying mechanism of Li metal electrodeposition behavior, which can be regarded as a powerful tool to help the community to understand the scientific challenges for filling the gaps. [ 7a,76 ] Following, the problematic issues of solid‐state batteries will be unrolled step by step.…”