调节凝胶聚合物电解质中的交联密度以抑制锂枝晶的产生

IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC ACS Applied Electronic Materials Pub Date : 2024-11-07 DOI:10.1021/acsaelm.4c0157310.1021/acsaelm.4c01573
Huashuo Jin, Wei Hao, Cancan Zhang*, Feng Yu* and Yong Chen*, 
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引用次数: 0

摘要

高理论容量和低电化学电位使金属锂成为最有希望取代石墨负极的材料。然而,锂枝晶的生长是限制锂金属电池发展的关键问题。作为一种固态电解质,凝胶聚合物电解质(GPE)与液态电解质相比具有一定的抑制锂枝晶生长的能力,但其抑制机理并不十分明确。在这项工作中,我们通过调节 GPE 的交联密度,验证了交联的 GPE 网络对锂离子的溶解结构有一定的影响。GPE 交联密度的增加会诱导出以接触离子对/溶剂分离离子对和 Li+ 聚集物为主的 Li+ 溶出鞘,有利于形成稳定的富含 LiF 的 SEI,从而抵御锂枝晶的产生。基于高交联 GPE 的磷酸铁锂全电池在 0.2C 速率下循环 220 次后仍能保持 81.9% 的高容量保持率,在 0.5C 速率下循环 140 次后仍能保持 90.1%的高容量保持率。首次描述了交联 GPE 对锂枝晶的抑制机制,为 GPE 的设计提供了更好的思路。
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The Modulation of Cross-Linking Density in Gel Polymer Electrolyte for the Inhibition of Lithium Dendrite

The high theoretical capacity and low electrochemical potential make lithium metal the most promising material to replace the graphite anode. However, lithium dendrite growth is the key problem that limits the development of lithium metal batteries. As a solid electrolyte, the gel polymer electrolyte (GPE) possesses a certain ability to inhibit the growth of lithium dendrites compared with a liquid electrolyte, but the inhibition mechanism is not very clear. In this work, through the regulation of GPE cross-linking density, we verify that the cross-linked GPE network has a certain influence on the solvation structure of lithium ions. The increased cross-linking density of GPE induces the Li+ solvated sheath dominated by contact ion pairs/solvent-separated ion pairs and Li+ aggregates, which is conducive to the formation of stable LiF-rich SEIs to resist lithium dendrites. The high cross-linked GPE-based LiFePO4 full battery also exhibits a high capacity retention rate of 81.9% even after 220 cycles at a rate of 0.2C and 90.1% after 140 cycles at a rate of 0.5C. The inhibiting mechanism of lithium dendrites by the cross-linked GPE is described for the first time, which provides a better idea for the design of GPE.

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CiteScore
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期刊介绍: ACS Applied Electronic Materials is an interdisciplinary journal publishing original research covering all aspects of electronic materials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials science, engineering, optics, physics, and chemistry into important applications of electronic materials. Sample research topics that span the journal's scope are inorganic, organic, ionic and polymeric materials with properties that include conducting, semiconducting, superconducting, insulating, dielectric, magnetic, optoelectronic, piezoelectric, ferroelectric and thermoelectric. Indexed/​Abstracted: Web of Science SCIE Scopus CAS INSPEC Portico
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