Due to the rapidly increasing demands of lithium-ion batteries, it is imperative to develop separators and even solid-state electrolytes with high biocompatibility/biodegradability to increase their sustainable economic values. In this context, we develop a series of 2,2,6,6-tetramethylpiperidine-1-oxyl-oxidized cellulose nanofiber (TOCN)-embedded solid polymer electrolytes (SPEs) through an environmentally friendly one-pot, organic solvent-free manufacturing process, for which the natural TOCN acts as a rigid 3D skeleton and polyethylene glycol (PEG₃₃₅₀) acts as the soft matrix. Unlike typical inorganic fillers (e.g., Al₂O₃), the addition of a small amount of TOCN into PEG allows the formation of free-standing SPE films. In addition to greatly improving the mechanical strength, the introduced TOCN preserves sufficient ion transport channels. The optimized free-standing TP28 SPE membrane possesses a decent ionic conductivity of 4.89 × 10^–4 S cm^–1 associated with a t_Li+ value of 0.31 at 80 °C, a high electrochemical stability window of >4.0 V, and a high tensile strength of 1.10 MPa. It also exhibits effective functionality and compatibility with the Li-metal (Li-symmetric cell cycling over 900 h at 80 °C) anode and the LiFePO₄ cathode. The assembled all-solid-state LiFePO₄|TP28|Li battery delivers great rate capability and cycling performance (96.5% after 100 cycles) with an initial capacity of 151 mAh g^–1 at 0.1 C at 60 °C. Our results demonstrate the promising potential of lignocellulosic biomass for fabricating biocompatible SPEs for Li-metal batteries that can largely increase their sustainable economic values.

中文翻译：

---

用于全固态锂金属电池的2,2,6,6-四甲基哌啶-1-氧基氧化纤维素纳米纤维嵌入聚合物电解质

由于锂离子电池的需求迅速增长，开发具有高生物相容性/生物可降解性的隔膜甚至固态电解质以提高其可持续经济价值势在必行。在此背景下，我们通过环保一锅法、无有机溶剂制造开发了一系列2,2,6,6-四甲基哌啶-1-氧基氧化纤维素纳米纤维（TOCN）嵌入的固体聚合物电解质（SPE）该过程中，天然 TOCN 作为刚性 3D 骨架，聚乙二醇 (PEG ₃₃₅₀ ) 作为软基质。与典型的无机填料（例如 Al ₂ O ₃），在 PEG 中添加少量 TOCN 可以形成独立式 SPE 膜。除了大大提高机械强度外，引入的TOCN还保留了足够的离子传输通道。优化的独立式 TP28 SPE 膜具有 4.89 × 10 –4 ^S cm ^{–1的良好离子电导率（80 °C 时}t _Li+值为0.31）、>4.0 V 的高电化学稳定性窗口和高拉伸强度强度为1.10兆帕。它还表现出有效的功能以及与锂金属（80 °C 下锂对称电池循环超过 900 小时）阳极和 LiFePO ₄阴极的兼容性。组装好的全固态LiFePO ₄|TP28|锂电池具有出色的倍率性能和循环性能（100 次循环后为 96.5%）， 60 °C、0.1 C 时的初始容量为 151 mAh g ^{–1 。}我们的研究结果表明，木质纤维素生物质在制造用于锂金属电池的生物相容性固相萃取物方面具有巨大的潜力，可以大大提高其可持续经济价值。