Virtues of Cold Isostatic Pressing for Preparation of All-Solid-State-Batteries with Poly(Ethylene Oxide)

All-solid-state-batteries (ASSBs) necessitate the preparation of a solid electrolyte and an electrode couple with individually dense and compact structures with superior interfacial contact to minimize overall cell resistance. A conventional preparation method of solid polymer electrolyte (SPE) with polyethylene-oxide (PEO) generally consists in employing uni-axial hot press (HP) to densify SPE. However, while uni-axial press with moderate pressure effectively densifies PEO with Li salts, excessive pressure also unavoidably results in perpendicular elongation and deformation for polymer matrix. In this research, to overcome this limitation for the uni-axial press technique, a cold isostatic press (CIP) is applied to the fabrication of ASSB with PEO and LiFePO₄ . CIP effectively and uniformly applies pressure as high as 500 MPa without deformation. Characterizations confirm that CIP treated SPE has enhanced mechanical puncture strength, increasing from 499.3±22.6 to 539.3±22.6 g, and ionic conductivity, increasing from 1.04×10^-4 to 1.91×10^-4  S cm^-1 at 50 °C. ASSB treated by CIP demonstrates remarkably enhanced rate capability and cyclability compared with the cell processed by HP, which is further evidenced by improvement of the apparent Li ion diffusion constant based on Sand equation analysis. The improvement enabled by CIP treatment originates from the superior interface uniformity between electrodes and SPE and from the densification of the LiFePO₄ and SPE composite electrode.