Kim, Hyeyun Lee, Chaeeun Jo, Jaemin Yu, Seonmyeong Shin, Sunghee Hur, Kahyun Koo, Bonwook Kim, Kwang Ho Hwang, Jinyeon 2025-06-25T05:30:05Z 2025-06-25T05:30:05Z 2025-06-21 2025-08 0144-8617 https://pubs.kist.re.kr/handle/201004/152685 Multilayered porous separators consisting of cellulose nanofibers (CNF) and SiO2 coating are fabricated for lithium-ion batteries (LIBs) as an eco-friendly alternative to conventional polyolefin separators. Employing a sol-gel synthesis method, SiO2 nanoparticles are intricately arranged on CNF to create core-shell structured CNF-SiO2 composites. Simple binder-free CNF-SiO2 surface coated composite separators are obtained via alternating sequential vacuum filtration of CNF suspensions and the nanocomposite coating functional layers, resulting in bi- and tri-layered separators. CNF entangled structure determines the pore architecture of CNF-SiO2 as a molecular template, while simultaneously tailoring the size distribution of pores and fibers within the separator, thus optimizing Li-ion transport pathways. By combining core-shell structured CNF-SiO2 nanocomposites as a functional layer with CNF separators, the resulting multilayer separators significantly improve the electrochemical stability of LIBs due to the effective suppression of electrolyte decomposition and dendrite growth on the Li metal surface. This approach simplifies material sourcing and production processes, making it particularly attractive for large-scale manufacturing for LIBs separators from carbohydrate precursors extracted from biomass. This study highlights the potential of chemically modified cellulose-based nanostructures as high-performing upcycled separators for energy storage, resulting in their possible commercial applications. English Pergamon Press Ltd. Multilayered separators with core-shell structured nanocellulose-SiO2 nanocomposites for lithium-ion batteries Article 10.1016/j.carbpol.2025.123677 1 Carbohydrate Polymers, v.362 Carbohydrate Polymers 362 N scie scopus 001510217200001 Chemistry, Applied Chemistry, Organic Polymer Science Chemistry Polymer Science Article CELLULOSE ELECTROLYTE MECHANISM SIO2 Lithium-ion batteries Sustainable separators Cellulose nanofibers Nanocomposites Dendrite inhibition