Rasupillai Dharmaraj, VasantanVasantanRasupillai DharmarajSarkar, AyanAyanSarkarWu, Yueh-AnYueh-AnWuChen, Han-ChenHan-ChenChenLin, Yu-PingYu-PingLinChung, Ren-JeiRen-JeiChungLiu, Ru-ShiRu-ShiLiu2025-06-302025-06-302025https://scholars.lib.ntu.edu.tw/handle/123456789/730365Anode modification is vital for enhancing the performance and lifespan of Mg-O2 batteries. This study presents an AlCl3/PTHF coating process to improve the stability of magnesium anodes. The coating, which is formed by treating the Mg metal with an AlCl3 and tetrahydrofuran (THF) solution, creates a gradient hybrid layer with a PTHF-rich top for facilitating Mg-ion transport and a magnesiophilic Al-Mg mixed ionic conductive surface for uniform Mg plating and stripping. The AlCl3/PTHF-coated anode achieved remarkable stability, cycling for over 300 h in symmetric Mg-Mg cells with markedly reduced overpotential compared with bare Mg anodes. Integrated with electrospun-quasi-solid-state electrolytes (EQSSEs) and Ru/CNT cathodes in Mg-O2 cells, the modified anode demonstrated excellent compatibility, delivering stable performance for over 50 cycles under controlled discharge conditions. These findings indicate the synergistic benefits of the AlCl3/PTHF-coated Mg anode, EQSSE, and Ru/CNT cathode, paving the way for sustainable high-performance Mg-O2 battery systems.en[SDGs]SDG7journal article10.1039/d5ta00476d