Designing Compatible Ceramic/Polymer Composite Solid‐State Electrolyte for Stable Silicon Nanosheet Anodes

Abstract

The commercialization of silicon anode for lithium‐ion batteries has been hindered by severe structure fracture and continuous interfacial reaction against liquid electrolytes, which can be mitigated by solid‐state electrolytes. However, rigid ceramic electrolyte suffers from large electrolyte/electrode interfacial resistance, and polymer electrolyte undergoes poor ionic conductivity, both of which are worsened by volume expansion of silicon. Herein, by dispersing Li1.3Al0.3Ti1.7(PO4)3 (LATP) into poly(vinylidene fluoride)‐hexafluoropropylene (PVDF‐HFP) and poly(ethylene oxide) (PEO) matrix, the PVDF‐HFP/PEO/LATP (PHP‐L) solid‐state electrolyte with high ionic conductivity (1.40 × 10−3 S cm−1), high tensile strength and flexibility is designed, achieving brilliant compatibility with silicon nanosheets. The chemical interactions between PVDF‐HFP and PEO, LATP increase amorphous degree of polymer, accelerating Li+ transfer. Good flexibility of the PHP‐L contributes to adaptive structure variation of electrolyte with silicon expansion/shrinkage, ensuring swift interfacial ions transfer. Moreover, the solid membrane with high tensile limits electrode structural degradation and eliminates continuous interfacial growth to form stable 2D solid electrolyte interface (SEI) film, achieving superior cyclic performance to liquid electrolytes. The Si//PHP‐L15//LiFePO4 solid‐state full‐cell exhibits stable lithium storage with 81% capacity retention after 100 cycles. This work demonstrates the effectiveness of composite solid electrolyte in addressing fundamental interfacial and performance challenges of silicon anodes.

Facile construction of flower-like MoO2/MoS2 heterostructures encapsulated in nitrogen-doped carbon for high-performance sodium-ion storage

“…The low ICE value is mainly attributed to irreversible capacity loss originating from the decomposition of the electrolyte and generation of SEI layers. 61,62 Fig. 3c exhibits the rate properties of MoO 2 / MoS 2 @NC, MoO 2 /MoS 2 , MoO 2 @NC, and MoS 2 .…”

Electrodeposition of Silicon Fibers from KI–KF–KCl–K2SiF6 Melt and Their Electrochemical Performance during Lithiation/Delithiation

“…Therefore, the behavior of the obtained silicon fibers should be studied with other electrolytes and structural materials. In particular, many works studied both the performance of silicon anodes with solid and polymer electrolytes [28][29][30] and the performance of mixtures of silicon of different morphologies with graphite [31,32], oxides [33,34], carbides, and other materials [35].…”

“…Therefore, the behavior of the obtained silico fibers should be studied with other electrolytes and structural materials. In particula many works studied both the performance of silicon anodes with solid and polymer elec trolytes [28][29][30] and the performance of mixtures of silicon of different morphologies wit graphite [31,32], oxides [33,34], carbides, and other materials [35]. In addition to increased energy costs, a significant value of irreversible capacitance leads to irreversible loss of part of the lithium ions, both in the electrolyte and in the cathode material.…”