Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators
Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators
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DOI：
10.3390/batteries8120253
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发表时间：
2022-11
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影响因子：
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通讯作者：
Daniel A. Gribble;Zih-Yu Lin;Sourav Ghosh;B. Savoie;V. Pol
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作者：
Daniel A. Gribble;Zih-Yu Lin;Sourav Ghosh;B. Savoie;V. Pol
高能量密度锂硫电池（LSBs）是锂离子电池（LIBs）的潜在替代品。然而，实际寿命受到多硫化锂（LiPS）穿梭的抑制。与此同时，全球塑料垃圾的积累威胁着我们的生态系统。本文研究了一种快速简便的将聚对苯二甲酸乙二醇酯（PET）废弃物转化为有用材料的方法。以废汽水瓶为原料，经微波解聚制备对苯二甲酸二酯（Li2TP）和对苯二甲酸二钾（K2TP）盐，并将溶液涂布在玻璃纤维纸（GFP）分离器上。含有Li2TP@GFP和K2TP@GFP的盐功能化分离器减轻了LiPS的穿梭并改善了电池中的电化学性能。孔隙分析和密度泛函理论（DFT）计算表明，其作用机制是通过与大量羧酸基的静电相互作用协同物理阻断纳米孔中体积较大的LiPS阴离子和扩散抑制。与未修饰的GFP相比，含有K2TP@GFP分离器的LSBs具有最高的LiPS亲和力和最小的孔径，其初始容量增加了5.4%，达到648 mAh g - 1，循环100次容量增加了23%，达到551 mAh g - 1。总体而言，K2TP@GFP在100次循环后保留了85%的初始容量，平均每循环容量衰减0.15%。相比之下，GFP在100次循环后仅保留了73%的初始容量，平均容量损失0.27%，证明了有效的lip保留。
High energy density lithium–sulfur batteries (LSBs) are a potential replacement for lithium-ion batteries (LIBs). However, practical lifetimes are inhibited by lithium polysulfide (LiPS) shuttling. Concurrently, plastic waste accumulation worldwide threatens our ecosystems. Herein, a fast and facile strategy to upcycle polyethylene terephthalate (PET) waste into useful materials is investigated. Dilithium terephthalate (Li2TP) and dipotassium terephthalate (K2TP) salts were synthesized from waste soda bottles via microwave depolymerization and solution coated onto glass fiber paper (GFP) separators. Salt-functionalized separators with Li2TP@GFP and K2TP@GFP mitigated LiPS shuttling and improved electrochemical performance in cells. Pore analysis and density functional theory (DFT) calculations indicate the action mechanism is synergistic physical blocking of bulky LiPS anions in nanopores and diffusion inhibition via electrostatic interactions with abundant carboxylate groups. LSBs with K2TP@GFP separator showing highest LiPS affinity and smallest pore size demonstrated enhanced initial capacity as compared to non-modified GFP by 5.4% to 648 mAh g−1, and increased cycle 100 capacity by 23% to 551 mAh g−1. Overall, K2TP@GFP retained 85% of initial capacity after 100 cycles with an average capacity fading of 0.15% per cycle. By comparison, GFP retained only 73% of initial capacity after 100 cycles with 0.27% average capacity loss, demonstrating effective LiPS retention.