Kim Seungwon, Park Sewon, Kim Minjee, Cho Yoonhan, Kang Gumin, Ko Sunghyun, Yoon Daebong, Hong Seungbum, Choi Nam-Soon
Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, Republic of Korea.
Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, Republic of Korea.
Adv Sci (Weinh). 2025 Jan;12(3):e2411466. doi: 10.1002/advs.202411466. Epub 2024 Nov 22.
The solid-electrolyte interphase (SEI) is a key element in anode-electrolyte interactions and ultimately contributes to improving the lifespan and fast-charging capability of lithium-ion batteries. The conventional additive vinyl carbonate (VC) generates spatially dense and rigid poly VC species that may not ensure fast Li transport across the SEI on the anode. Here, a synthetic additive called isosorbide 2,5-dimethanesulfonate (ISDMS) with a polar oxygen-rich motif is reported that can competitively coordinate with Li ions and allow the entrance of PF anions into the core solvation structure. The existence of ISDMS and PF in the core solvation structure along with Li ions enables the movement of anions toward the anode during the first charge, leading to a significant contribution of ISDMS and LiPF to SEI formation. ISDMS leads to the creation of ionically conductive and electrochemically stable SEI that can elevate the fast-charging performance and increase the lifespan of LiNiCoMnO (NCM811)/graphite full cells. Additionally, a sulfur-rich cathode-electrolyte interface with a high stability under elevated-temperature and high-voltage conditions is constructed through the sacrificial oxidation of ISDMS, thus concomitantly improving the stability of the electrolyte and the NCM811 cathode in a full cell with a charge voltage cut-off of 4.4 V.
固体电解质界面(SEI)是阳极与电解质相互作用的关键因素,最终有助于提高锂离子电池的使用寿命和快速充电能力。传统添加剂碳酸亚乙烯酯(VC)会生成空间致密且刚性的聚VC物种,这可能无法确保锂离子在阳极上的SEI中快速传输。在此,报道了一种名为异山梨醇2,5-二甲磺酸酯(ISDMS)的合成添加剂,其具有富含极性氧的结构单元,能够与锂离子竞争性配位,并使PF阴离子进入核心溶剂化结构。核心溶剂化结构中ISDMS和PF与锂离子共存,使得阴离子在首次充电期间向阳极移动,从而对SEI的形成有显著贡献。ISDMS导致形成离子导电且电化学稳定的SEI,可提升快速充电性能并延长LiNiCoMnO(NCM811)/石墨全电池的使用寿命。此外,通过ISDMS的牺牲氧化构建了在高温和高压条件下具有高稳定性的富硫阴极-电解质界面,从而同时提高了全电池中电解质和NCM811阴极在充电截止电压为4.4 V时的稳定性。