3D Printed P(VdF‐HFP)/SBA‐15 composite‐based gel polymer electrolyte versus commercial celgard: A comparative investigation on thermal stability and electrochemical performance for lithium‐ion battery application

Abstract The current work reports on tailoring of 3D printed gel polymer electrolyte (GPE) employing poly(vinylidene fluoride‐co‐hexafluoropropylene) P(VdF‐HFP) as the host matrix and mesoporous Santa Barbara Amorphous‐15 (SBA‐15) mesoporous sieve as ceramic filler. Further, this work envisages an investigation on its physicochemical properties, thermal shrinkage behavior, and electrochemical performance. An effort has been undertaken to formulate 3D printable P(VdF‐HFP)/SBA‐15 composite‐based GPE ink with suitable rheological properties. The breath figure method is followed to investigate the influence of 1‐methyl‐2‐pyrrolidinone (NMP)/tetrahydrofuran (THF) mixture as a solvent on the porosity of 3D printed GPE, through which enhanced porosity is evident from scanning electron microscopy (SEM) analysis. The morphological analysis further confirms the hybrid porous structure facilitated by the addition of SBA‐15 into the P(VdF‐HFP) matrix. The 3D printed P(VdF‐HFP)/SBA‐15 (10%) composite‐based GPE shows promising ionic conductivity in the order of 0.2 × 10 −4 S/cm at room temperature and demonstrates excellent dimensional thermal stability up to 175°C. The electrochemical measurement of 3D printed GPE is tested separately using 3D printed cathode half‐cell (3D printed LFP vs. Li + ) and 3D printed anode half cell (3D printed LTO vs. Li + ) with GPE as separator. Further, also tested with conventionally prepared electrode and the coin cell studies show discharge capacity of 3D printed P(VdF‐HFP)/SBA‐15 (10%) composite‐based GPE is comparable to commercial celgard separator. All these features speculate that the 3D printed fabricated in the current work may find potential application in lithium‐ion battery.