Zheng Ruijie, Kobayashi Shigeru, Ogawa Mana, Katsuragawa Hiroto, Watanabe Yuki, Deng Jun, Nakayama Ryo, Nishio Kazunori, Shimizu Ryota, Tateyama Yoshitaka, Moriya Makoto, Hitosugi Taro
School of Materials and Chemical Technology, Institute of Science Tokyo, Tokyo 152-8552, Japan.
Department of Chemistry, The University of Tokyo, Tokyo 113-0033, Japan.
ACS Appl Mater Interfaces. 2025 Apr 9;17(14):21951-21957. doi: 10.1021/acsami.4c22076. Epub 2025 Mar 28.
Molecular crystals composed of lithium bis(fluorosulfonyl)amide (LiFSA) and succinonitrile (SN), hereafter referred to as Li(FSA)(SN), are a promising solid electrolyte. To realize a wider application of molecular crystal solid electrolytes, it is critical to investigate the interface of Li(FSA)(SN) and 5 V-class positive electrodes. Here, we studied the interface of Li(FSA)(SN) with 5 V-class LiNiMnO (LNMO) positive electrodes utilizing modeled thin-film batteries. The Li(FSA)(SN)|LNMO interfaces degrade, leading to an increase in interface resistance and capacity loss. By inserting an amorphous LiPO layer into the Li(FSA)(SN)|LNMO interface, the low interface resistance remains, and no interphase layer is observed. The discharge capacity remains at 96% after 100 charge and discharge cycles. This study demonstrated the feasibility of operating Li(FSA)(SN) in a 5 V-class solid-state battery revealing the potential of molecular crystal solid electrolytes in high-energy-density batteries.
由双（氟磺酰）亚胺锂（LiFSA）和丁二腈（SN）组成的分子晶体，以下简称Li(FSA)(SN)，是一种很有前景的固体电解质。为了实现分子晶体固体电解质更广泛的应用，研究Li(FSA)(SN)与5V级正极的界面至关重要。在此，我们利用模拟薄膜电池研究了Li(FSA)(SN)与5V级LiNiMnO（LNMO）正极的界面。Li(FSA)(SN)|LNMO界面会退化，导致界面电阻增加和容量损失。通过在Li(FSA)(SN)|LNMO界面插入非晶态LiPO层，低界面电阻得以保持，且未观察到中间相层。经过100次充放电循环后，放电容量仍保持在96%。这项研究证明了在5V级固态电池中使用Li(FSA)(SN)的可行性，揭示了分子晶体固体电解质在高能量密度电池中的潜力。
