Pathway to High Rate Capability in Interconnected Composite Electrolytes: A Case Study with a Single-Ion-Conducting Polymer

IF 5.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL
Ritu Sahore*, Kyra D. Owensby, Beth L. Armstrong, Jiyoung Ock, Michelle L. Lehmann, Andrew M. Ullman, Sergiy Kalnaus* and Xi Chelsea Chen*, 
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Abstract

In a three-dimensional interconnected polymer/ceramic composite electrolyte (3D composite), both the polymer and ceramic electrolyte phases are individually connected with a polymer-rich surface layer to provide conformal contact with the electrodes. This work investigates how the transference number of the polymer phase affects the electrochemical properties of the 3D composite. Here, we fabricate a 3D composite using a “single-ion” conducting polymer electrolyte (PE), Li1+x+yAlxTi2–xSiyP3–yO12 (LICGC) ceramic, and compare its electrochemical properties with the neat polymer, and with a 3D composite made with a dual-ion-conducting PE (we reported previously). Our results reveal that changing the polymer phase from a dual-ion-conducting PE to a single-ion-conducting PE results in a 9-fold increase in the limiting current density, although the interfacial impedance between the polymer and LICGC ceramic remains high (and contributes significantly to the total impedance of the 3D composite). The limiting current density of the 3D composite is dictated by the PE and minimally affected by the ceramic scaffold. The ceramic scaffold, however, helps to ease the concentration gradient buildup within the PE and moderately improves the overall transference number. The LICGC scaffold does not provide any additional Li dendrite resistance due to its high reactivity with Li.

Abstract Image

互联复合电解质的高倍率性能途径:以单离子导电聚合物为例
在三维互联聚合物/陶瓷复合电解质(3D复合)中,聚合物和陶瓷电解质相分别与富含聚合物的表面层连接,以提供与电极的保形接触。这项工作研究了聚合物相的转移数如何影响三维复合材料的电化学性能。在这里,我们使用“单离子”导电聚合物电解质(PE), Li1+x+ yAlxTi2-xSiyP3-yO12 (LICGC)陶瓷制作了3D复合材料,并将其电化学性能与纯聚合物和双离子导电PE制成的3D复合材料(我们之前报道过)进行了比较。我们的研究结果表明,将聚合物相从双离子导电PE转变为单离子导电PE导致极限电流密度增加9倍,尽管聚合物和LICGC陶瓷之间的界面阻抗仍然很高(并且对3D复合材料的总阻抗有很大贡献)。3D复合材料的极限电流密度由PE决定,并且受陶瓷支架的影响最小。然而,陶瓷支架有助于缓解PE内浓度梯度的积聚,并适度提高总体转移数。由于其与锂的高反应性,LICGC支架不提供任何额外的锂枝晶电阻。
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来源期刊
ACS Applied Energy Materials
ACS Applied Energy Materials Materials Science-Materials Chemistry
CiteScore
10.30
自引率
6.20%
发文量
1368
期刊介绍: ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. 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, engineering, physics, bioscience, and chemistry into important energy applications.
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