Highly conductive and mechanically robust composite cathodes based on 3D interconnected elastomeric networks for deformable lithium‐ion batteries

Deformable lithium‐ion batteries (LIBs) can serve as the main power sources for flexible and wearable electronics owing to their high energy capacity, reliability, and durability. The pivotal role of cathodes in LIB performance necessitates the development of mechanically free‐standing and stretchable cathodes. This study demonstrates a promising strategy to generate deformable cathodes with electrical conductivity by forming 3D interconnected elastomeric networks. Beginning with a physically crosslinked polymer network using poly(vinylidene fluoride‐co‐hexafluoropropylene) and 1‐ethyl‐3‐methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMI][TFSI]), subsequent exchange with a 1 M LiPF6 electrolyte imparts elastic characteristics to the cathodes. The resulting LiFePO4 composite electrodes maintained their resistance under 500 consecutive bending cycles at an extremely small bending radius of 1.8 mm and showed high discharge capacity of 158 mAh g−1 with stable potential plateaus in charging and discharging curves. Moreover, flexible cells utilizing the composite electrodes exhibited superior operational stability under rolling, bending, and folding deformations. Deformable LiFePO4 cathodes with superior electrical conductivity were developed by forming 3D interconnected elastomeric networks in composite electrodes. The deformable cathodes maintained electrical conductivity even under 500 consecutive bending cycles at an extremely small bending radius of 1.8 mm and the flexible pouch cells utilizing the composite electrodes successfully delivered electrical power to an light‐emitting diode when subjected to bending, rolling, and folding conditions.