Publication date: 10th April 2024
Li(FSA)(SN)2 molecular crystal solid electrolytes, consisting of lithium bis-(fluorosulfonyl)imide (LiFSA) and succinonitrile (SN), exhibit comparable ionic conductivity (1.1×10-4 S·cm-1) and improved transference number (0.95) with traditional solid polymer electrolytes [1]. FSA anions in an ionic liquid electrolyte contribute to the passivation layer formed on the positive electrode surface [2], suggesting that Li(FSA)(SN)2 may enable battery operation under high voltage by passivating the interface. However, the adaptability of Li(FSA)(SN)2 solid electrolytes in high-voltage operation is still unclear. In this study, we fabricated a battery using a thin-film 5 V-class LiNi0.5Mn1.5O4 (LNMO) positive electrode and investigated the operation of the battery under high voltages.
In the early cycles, the battery composed of Li(FSA)(SN)2 and LNMO shows successful charge and discharge cycles up to 4.8 V vs. Li/Li+. However, the capacity shows severe degradation (54% after 100 cycles with the current density of 10 μA·cm-2). Continuous interfacial side reactions and thick interphase layer formation at the Li(FSA)(SN)2 | LNMO interface may have led to capacity degradation. An insufficient passivation of the interface is suggested. Therefore, a highly stable amorphous Li3PO4 buffer layer was inserted on the Li(FSA)(SN)2 | LNMO interface to passivate the interface. With the insertion of Li3PO4, the capacity degradation was suppressed to 4% after 100 charge-discharge cycles, indicating that the insertion of Li3PO4 stabilized the interface even at a high voltage of 4.8 V vs. Li/Li+. This study reveals the potential of molecular crystal solid electrolytes for 5 V-class all-solid-state batteries and highlights the importance of interfacial engineering on battery performance.
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