Abstract: Calendering is a crucial step in lithium-ion battery (LIB) electrode manufacturing, as it strongly influences electrode microstructure, mechanical integrity, and electrochemical behavior. This study introduces an innovative induction heating-assisted calendering (IHAC) technique that enables non-contact, directional heating of the current collector, allowing precise thermal control and microstructural tailoring during compaction. The effects of IHAC on the thickness, morphology, interfacial adhesion, and impedance of LiFePO4 electrodes were systematically investigated, and the processed electrodes were further evaluated electrochemically. Discrete element simulations revealed that IHAC produces a surface porosity of 36.5% and an internal porosity of 27.3%, corresponding to a 36.7% enhancement in surface porosity compared with conventional calendering. This graded pore structure was validated by scanning electron microscopy. Within the temperature range of 25–130 °C, IHAC substantially improved electrode properties and electrochemical performance. At an optimal temperature of 70 °C, the IHAC-processed electrode exhibited a thickness of 189.8 μm, a peel force of 13.3 N m−1, a resistance of 7.41 Ω·cm, a 2C discharge capacity of 142.4 mAh/g, and a cycle life of 267 cycles at 90% capacity retention. In comparison, the HC electrode under the same condition measured 189 μm, 12.2 N m−1, 7.33 Ω·cm, 139.8 mAh/g, and 251 cycles. Moreover, relative to conventional calendering at 25 °C, the IHAC-processed electrode achieved a 1.65% reduction in thickness, a 26.7% improvement in adhesion, a 7.7% decrease in resistance, a 2% increase in 2C discharge capacity, and a 40% extension in cycle life. These improvements arise from a “hot-core/cold-surface” thermal gradient that induces plastic deformation in the electrode interior while maintaining surface elasticity. Upon cooling, a functionally graded microstructure forms, featuring a porous surface and dense core, which enhances both energy and power performance. These findings highlight the critical role of thermal gradient directionality in determining electrode architecture and demonstrate IHAC as a promising pathway for the synergistic enhancement of volumetric energy and power density in LIBs. Owing to its non-contact operation, high efficiency, and cost-effectiveness, IHAC offers a practical and scalable solution for advanced battery manufacturing and contributes a new approach to more sustainable battery production globally.
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