Heo, Yeong Hoon Yoon, Juhee Park, Minhyuck Kim, Do Hyun Hyun, Jong Chan Kim, Sion Park, Jimin Kim, Jisoo Ha, Son Yeon, Jiyun Lee, Jeonghun Jin, Hyoung-joon Lim, Hyung-kyu Yun, Young Soo 2026-02-19T05:30:38Z 2026-02-19T05:30:38Z 2026-02-19 2026-01 https://pubs.kist.re.kr/handle/201004/154304 Despite the high theoretical volumetric capacity of aluminum metal anodes (AMAs), their practical use in rechargeable aluminum batteries (RABs) is hindered by low capacity utilization and short-circuit-induced cell failure. Herein, we investigate the aluminum nucleation and growth behavior on a 2D electrode platform to uncover the origins of such failures, integrating experimental analysis with theoretical calculations. We find that the failure capacity is strongly dependent on separator thickness, irrespective of separator type. Short-circuiting arises from unfavorable multi-step reactions, where inefficient Cl− removal promotes vertical Al growth due to localized accumulation of reaction products. Based on these insights, we design a 3D nanostructured graphitic carbon electrode (3D-GCE) to mitigate local AlCl4− buildup and enhance Al reversibility. Additionally, a Cl-doped polypropylene (Cl-PP) separator is employed to facilitate Cl− transport via the Grotthuss mechanism. This integrated design achieves a record capacity of ~8.2 mAh cm−2 and stable cycling over 500 cycles with a single thin PP separator. English Wiley Suppressing vertical aluminum growth via accelerated interfacial Cl− dynamics for high-areal-capacity, long-life aluminum metal anodes Article 10.1002/inf2.70113 1 InfoMat InfoMat Y scie 2-s2.0-105029058104 Materials Science, Multidisciplinary Materials Science Article; Early Access ELECTRICAL ENERGY-STORAGE IONIC LIQUIDS LITHIUM BATTERY LIMITS 3D nanostructured graphitic carbon electrode aluminum metal anode aluminum nucleation and growth behavior cell-failure mechanism Cl-doped polypropylene separator high volumetric energy density rechargeable aluminum batteries