Song Hyunsub, Lee Jiyoung, Sagong Mingyu, Jeon Jiwon, Han Yeji, Kim Jinuk, Jung Hun-Gi, Yu Ji-Sang, Lee Jinwoo, Kim Il-Doo
Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, Republic of Korea.
Department of Chemical and Biological Engineering, Northwestern University, Evanston, IL, 60208, USA.
Adv Mater. 2024 Nov;36(47):e2407381. doi: 10.1002/adma.202407381. Epub 2024 Sep 1.
Construction of a robust artificial solid-electrolyte interphase (SEI) layer has proposed an effective strategy to overcome the instability of the lithium (Li). However, existing artificial SEI layers inadequately controlled ion distribution, leading to dendritic growth and penetration. Furthermore, the environmental impact of the manufacturing process and materials of the artificial layer is often overlooked. In this work, a chemically and physically reinforced membrane (C-Li@P) composed of the biocompatible Li coordinated carboxymethyl guar gum (CMGG) and polyacrylamide (PAM) polymers serves as an artificial SEI membrane for dendrite-free Li. This membrane with hollow channels not only directs ion flux along the interspace of fibers, fostering uniform Li plating but also induces a desirable interface chemistry. Consequently, artificial SEI membrane-covered Li exhibits stable electrochemical plating/stripping reactions, surpassing the cycle life of ≈750% of bare Li. It demonstrates exceptional capacity retention of ≈93.9%, ≈88.1%, and ≈79.18% in full cells paired with LiNiMnCoO (NMC811), LiNiMnCoO (NMC622) and S cathodes, respectively over 200 cycles at 1 C rate. Additionally, the water-based green manufacturing and biodegradability of the membrane demonstrated the sustainable development and disposal of electrodes. This work provides a comprehensive framework for the design of an artificial layer chemically and physically regulating dendritic growth.
构建坚固的人工固体电解质界面(SEI)层提出了一种克服锂(Li)不稳定性的有效策略。然而,现有的人工SEI层对离子分布的控制不足,导致枝晶生长和穿透。此外,人工层制造工艺和材料对环境的影响常常被忽视。在这项工作中,由生物相容性锂配位羧甲基瓜尔胶(CMGG)和聚丙烯酰胺(PAM)聚合物组成的化学和物理增强膜(C-Li@P)用作无枝晶锂的人工SEI膜。这种具有中空通道的膜不仅引导离子通量沿着纤维间隙流动,促进锂的均匀沉积,还能诱导理想的界面化学性质。因此,覆盖有人工SEI膜的锂表现出稳定的电化学沉积/剥离反应,其循环寿命超过裸锂约750%。在与锂镍锰钴氧化物(NMC811)、锂镍锰钴氧化物(NMC622)和硫阴极配对的全电池中,在1 C倍率下经过200次循环后,它分别表现出约93.9%、约88.1%和约79.18%的出色容量保持率。此外,该膜的水基绿色制造工艺和生物可降解性证明了电极的可持续发展和处置。这项工作为设计化学和物理调节枝晶生长的人工层提供了一个全面的框架。