Blending Poly(ethylene oxide) and Li6.4La3Zr1.4Ta0.6O12 by Haake Rheomixer without any solvent: A low-cost manufacture method for mass production of composite polymer electrolyte

Composite solid electrolytes (CSEs) are considered as one of the important candidates for solid-state batteries . The conventional solvent-cast method that using an organic solvent to disperse polymer and ceramic particles has high cost and low efficiency. The agglomeration of ceramic particles in the solution and the residual solvent in CSEs also have side effects on the performance of the solid-state battery. A new technique to prepare composite solid electrolytes by internal-mix method to blend ceramic particles and polymers without any solvent has been proposed in this article. To contrastively study the internal-mix and solvent-cast methods, CSE samples with 50 wt% Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) and 50 wt% PEO polymer were prepared by the two methods and characterized by XRD , SEM, FTIR TG-DTA and DSC . The internal-mix process is free of any solvent, and thus no agglomeration or solvent remain in the polymer matrix . CSE prepared by the internal-mix process has less undesired Li 2 CO 3 and no residual solvent, thus exhibiting better thermal and electrochemical stability. All-solid-state battery with CSE prepared by internal-mix shows improved cycle performance than that prepared by solvent-cast. Environmentally friendly and low-cost preparation of PEO-based CSEs could be realized with the internal-mix method, and this technique is suitable for large-scale manufacture.