Wang Fei, Lu Anbang, Liu Zhendong, Zhang Weidong, Gao Yulin, Zhao Qi, Sun Jianguo, Zhang Chengzhi, Liu Quanbing, Liu Hongbo, Wang John
Department of Materials Science and Engineering, National University of Singapore, Singapore, 117574, Republic of Singapore.
Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology, College of Materials Science and Engineering, Hunan University, Changsha, 410082, China.
Adv Mater. 2025 Aug 27:e09207. doi: 10.1002/adma.202509207.
Sluggish solid-state diffusion kinetics of lithium ions is among the primary bottlenecks limiting the fast-charging performance of graphite anodes. Pre-intercalating molecules in graphite interlayers can tune the valence π-electrons, but there are few systematic studies in designing such structures by electron coupling to optimize the charge transfer kinetics. Herein, deliberately guided by simulations, the present study identifies and develops a class of electron-acceptor aluminum chloride species for intercalation into graphite (AC-G), aiming to accelerate lithium ions charge transfer to the intercalated graphite through the formation of electron-acceptor bridges within the graphite interlayers. Consequently, the AC-G achieves a two-order-of-magnitude enhancement in lithium ions diffusion coefficient (5.85 × 10 cm s) compared to that in pristine graphite. It delivers stable cycling over 2000 cycles with a high areal capacity retention of 3.84 mAh cm at 1C and maintains 500-cycle stability at 5C. Furthermore, an Ah-level pouch cell assembled with AC-G and cathode achieves an energy density of 285 Wh kg at 3C. The present work provides a new design strategy for graphite by introducing interlayer electron-bridging structures, offering valuable insights for next-generation fast-charging lithium-ion batteries.
锂离子缓慢的固态扩散动力学是限制石墨负极快速充电性能的主要瓶颈之一。在石墨层间预嵌入分子可以调节价π电子,但通过电子耦合设计此类结构以优化电荷转移动力学的系统研究较少。在此,本研究在模拟的有意指导下,识别并开发了一类用于嵌入石墨的电子受体氯化铝物种(AC-G),旨在通过在石墨层间形成电子受体桥来加速锂离子向嵌入石墨的电荷转移。因此,与原始石墨相比,AC-G的锂离子扩散系数提高了两个数量级(5.85×10 cm²/s)。它在1C下可稳定循环超过2000次,具有3.84 mAh/cm²的高面积容量保持率,在5C下保持500次循环稳定性。此外,用AC-G和正极组装的Ah级软包电池在3C下实现了285 Wh/kg的能量密度。本工作通过引入层间电子桥结构为石墨提供了一种新的设计策略,为下一代快速充电锂离子电池提供了有价值的见解。