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研究聚（3,4-乙撑二氧噻吩）：聚苯乙烯磺酸盐粘合剂作为锂硫电池硫阴极中的能量扩展剂

Investigating PEDOT:PSS Binder as an Energy Extender in Sulfur Cathodes for Li-S Batteries.

作者信息

Dent Matthew, Grabe Sean, Ayere Obehi, Babar Shumaila, Masteghin Mateus G, Cox David C, Howlin Brendan J, Baker Mark A, Lekakou Constantina

机构信息

Center for Engineering Materials, School of Mechanical Engineering Sciences, University of Surrey, Guildford, Surrey GU2 7XH, U.K.

Advanced Technology Institute, University of Surrey, Guildford, Surrey GU2 7XH, U.K.

出版信息

ACS Appl Energy Mater. 2024 Aug 26;7(17):7349-7361. doi: 10.1021/acsaem.4c01553. eCollection 2024 Sep 9.

DOI:10.1021/acsaem.4c01553
PMID:39268392
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11388141/
Abstract

Although lithium-sulfur (Li-S) batteries offer a high theoretical energy density, shuttling of dissolved sulfur and polysulfides is a major factor limiting the specific capacity, energy density, and cyclability of Li-S batteries with a liquid electrolyte. Cathode host materials with a microstructure to restrict the migration of active material may not totally eliminate the shuttling effect or may create additional problems that limit the full dissolution and redox conversion of all active cathode materials. Selecting a cathode coating binder with a multifunctional role offers a universal solution suitable for various cathode hosts. PEDOT:PSS is investigated as such a binder in this study via experimental testing and material characterization as well as multiscale modeling. The study is based on Li-S cells with a sulfur cathode in hollow porous particles as the cathode host and the 10 wt % PEDOT:PSS binder and electrolyte 1 M LiTFSI in 1:1 DOL:DME 1:1 v/v. A reference supercapacitor cell with the same electrolyte and electrodes comprising a coating of the same hollow porous particles and 10 wt % PEDOT:PSS revealed the pseudocapacitive effect of PEDOT:PSS following a surface redox mechanism that dominates the charge phase, which is equivalent to the discharge phase of the Li-S battery cell. A multipore continuum model for supercapacitors and Li-S cells is extended to incorporate the pseudocapacitive effects of PEDOT:PSS with the Li ions and the adsorption effects of PEDOT:PSS with respect to sulfur and lithium sulfides in Li-S cells, with the adsorption energies determined via molecular and simulations in this study. Experimental data and predictions of multiscale simulations concluded a 7-9% extension of the specific capacity of Li-S battery cells due to the surface redox effect of PEDOT:PSS and elimination of lithium sulfides from the anode by slowing down their migration and shuttling via their adsorption by the PEDOT:PSS binder.

摘要

尽管锂硫（Li-S）电池具有较高的理论能量密度，但溶解的硫和多硫化物的穿梭是限制具有液体电解质的Li-S电池的比容量、能量密度和循环稳定性的主要因素。具有微观结构以限制活性材料迁移的阴极主体材料可能无法完全消除穿梭效应，或者可能会产生其他问题，从而限制所有活性阴极材料的完全溶解和氧化还原转化。选择具有多功能作用的阴极涂层粘合剂提供了一种适用于各种阴极主体的通用解决方案。在本研究中，通过实验测试、材料表征以及多尺度建模，对PEDOT:PSS作为这种粘合剂进行了研究。该研究基于以中空多孔颗粒中的硫阴极作为阴极主体、10 wt% PEDOT:PSS粘合剂以及1 M LiTFSI的1:1 DOL:DME（1:1 v/v）电解质的Li-S电池。一个具有相同电解质和电极的参考超级电容器电池，其电极包括相同的中空多孔颗粒涂层和10 wt% PEDOT:PSS，揭示了PEDOT:PSS遵循在充电阶段占主导的表面氧化还原机制的赝电容效应，这与Li-S电池单元的放电阶段等效。将超级电容器和Li-S电池的多孔隙连续介质模型进行扩展，以纳入PEDOT:PSS与锂离子的赝电容效应以及PEDOT:PSS对Li-S电池中硫和硫化锂的吸附效应，其中吸附能在本研究中通过分子和模拟确定。实验数据和多尺度模拟的预测得出，由于PEDOT:PSS的表面氧化还原效应以及通过PEDOT:PSS粘合剂对硫化锂的吸附减缓其迁移和穿梭，Li-S电池单元的比容量提高了7 - 9%。

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