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In Operando Visualization of Polymerized Ionic Liquid Electrolyte Migration in Solid-State Lithium Batteries
ACS Energy Letters ( IF 19.3 ) Pub Date : 2024-12-19 , DOI: 10.1021/acsenergylett.4c02430 Bowen Chen, Ke Xu, Lingfei Tang, Qiang Li, Qi Chen, Liwei Chen
ACS Energy Letters ( IF 19.3 ) Pub Date : 2024-12-19 , DOI: 10.1021/acsenergylett.4c02430 Bowen Chen, Ke Xu, Lingfei Tang, Qiang Li, Qi Chen, Liwei Chen
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Polymerized ionic liquid (PIL) electrolytes with high flaming resistance, wide electrochemical stability window, and high flexibility have been widely explored for high safety, high energy density, and long-cycle lithium metal batteries (LMBs). Great efforts have been made in inhibiting anion movement in the PIL to increase the lithium transference number (tLi+), which reduces polarization loss and improves rate performance. However, the effect of tLi+ on the cycle performance is often overlooked because of self-limiting parasitic interfacial reactions involving anions. Here, PIL migration induced by mobile anions was visualized in operando via cross-sectional atomic force microscopy. Intense migration of the PIL with a low tLi+ breaks the interphase on electrodes and exacerbates anion decomposition, resulting in escalating interfacial impedance. The increased tLi+ inhibits interfacial electromechanical degradation and enhances cycle performance. This work reveals the pivotal but often unnoticed role of interfacial electro-mechanical coupling in PIL-based LMBs by taking advantages of in operando scrutiny of the buried interface.
更新日期：2024-12-20
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