탄소중립형 이차전지 실현을 위한 폐 분리막의 전기방사 기반 고기능 재활용 기술 연구
Development of Electrospinning-Based High-Performance Recycling Technology for Spent Battery Separators toward Carbon-Neutral Secondary Batteries
The rapid growth of electric vehicles and portable electronics has led to a significant increase in the consumption of lithium-ion batteries (LIBs). Consequently, a large number of spent batteries are being generated, posing serious environmental and resource challenges. Among the components of LIBs, separators—typically composed of polyolefin materials—are difficult to degrade and contribute to microplastic pollution when improperly disposed. However, these separators still retain a relatively intact physical structure after use, making them valuable candidates for recycling and reuse in next-generation energy storage systems. To address both environmental concerns and resource efficiency, this study explores a high-performance recycling strategy for spent LIB separators using electrospinning-based surface modification. Electrospinning offers several advantages, including low cost, high controllability of fiber morphology, and strong adhesion to substrate surfaces. It enables the fabrication of nanofiber layers with tunable porosity, mechanical strength, and wettability, which are crucial for restoring or even enhancing the performance of used separators. Experimental results show that spent separators exhibit a significant decline in high-rate (C-rate) discharge performance compared to fresh ones. Long-term usage appears to reduce the thickness of the separators, and their surfaces show signs of corrosion due to prolonged contact with battery electrolytes. FE-SEM analysis further reveals that the used separators consist of randomly distributed fibers with non-uniform diameters and surface contamination from particulate debris, indicating the necessity of targeted surface modification. Moreover, TGA results suggest that while thermal degradation is minimal below 100°C, decomposition begins at temperatures exceeding 100°C, highlighting the importance of future thermal resistance enhancement strategies. Based on our investigation of the fundamental physicochemical properties of spent separators, we propose an eco-friendly surface modification strategy utilizing electrospinning techniques. Specifically, we aim to coat the degraded separators using a composite nanofiber layer composed of biodegradable polyvinyl alcohol (PVA), recycled carbon fiber-reinforced polymer (rCFRP), and thermally stable aluminum oxide (Al₂O₃) additives. This surface treatment will be applied via electrostatic spraying methods, which allow uniform deposition and strong interfacial bonding. The incorporation of rCFRP enhances mechanical robustness, while Al₂O₃ improves thermal resistance, addressing the degradation issues observed in spent separators. This approach is expected to significantly improve the safety, durability, and reusability of separators in regenerated lithium-ion batteries, and contributes to the advancement of carbon-neutral and circular energy storage technologies.