Ma Chenyu, We Xinru, Feng Wenting, Ma Guanzhong, Yang Jianhang, Fan Shuhao, Sun Yiming, Wang Han, Liu Zihui, Han Junwei, Lv Wei, Kong Debin, Zhi Linjie
Shandong Key Laboratory of Advanced Electrochemical Energy Storage Technologies, College of New Energy, China University of Petroleum (East China), Qingdao 266580, China.
School of Materials Science and Engineering, China University of Petroleum (East China), Qingdao 266580, China.
ACS Nano. 2025 Sep 2;19(34):31213-31223. doi: 10.1021/acsnano.5c10334. Epub 2025 Aug 22.
Rechargeable metal-chlorine (Li/Na-Cl) batteries potentially have a high energy density, but the significant amount of electrolyte consumed to produce active metal chlorides for reversible chlorine conversion severely limits their real electrochemical performance. Herein, we use a cathode with precast metal chloride in the graphene layers as the initial active material to save the sacrificial electrolyte and deliver a fundamentally different start-up operation mode for metal-chlorine batteries. Furthermore, the metal chloride confined by the graphene layers achieves in situ confining conversion with gaseous chlorine during long cycling, causing substantially improved cathode kinetics in a lean electrolyte. With this cathode, both Li/Na-Cl batteries demonstrate higher capacity and prolonged cycling performance. Typically, the obtained Na-Cl batteries could deliver a high areal capacity (3 mAh cm) and stable life over 300 cycles under lean electrolyte conditions (20-60 μL). This work demonstrates the practical significance of utilizing a graphene interlayer to confine metal chloride as an initial active material for rechargeable alkali-metal-Cl batteries.
可充电金属氯（Li/Na-Cl）电池可能具有高能量密度，但为实现可逆氯转化而生产活性金属氯化物所消耗的大量电解质严重限制了其实际电化学性能。在此，我们使用石墨烯层中预制金属氯化物的阴极作为初始活性材料，以节省牺牲电解质，并为金属氯电池提供一种根本不同的启动操作模式。此外，被石墨烯层限制的金属氯化物在长时间循环过程中与气态氯实现原位限制转化，在贫电解质中使阴极动力学得到显著改善。使用这种阴极，Li/Na-Cl电池均展现出更高的容量和更长的循环性能。典型地，所制备的Na-Cl电池在贫电解质条件（20 - 60 μL）下可提供高面积容量（3 mAh cm）并在300次循环以上保持稳定寿命。这项工作证明了利用石墨烯夹层来限制金属氯化物作为可充电碱金属 - Cl电池初始活性材料的实际意义。
