Yoon Hana, Rezaee Mehdi, Lee Yeong A, Yim Kanghoon, Tamarany Rizcky, Lee Chan-Woo, McGraw Valerie S, Taniguchi Takashi, Watanabe Kenji, Kim Philip, Yoo Chung-Yul, Bediako D Kwabena
Energy Storage Laboratory, Korea Institute of Energy Research (KIER), Daejeon 34129, Republic of Korea.
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States.
Nano Lett. 2022 Feb 23;22(4):1726-1733. doi: 10.1021/acs.nanolett.1c04832. Epub 2022 Feb 8.
A rechargeable aluminum-ion battery based on chloroaluminate electrolytes has received intense attention due to the high abundance and chemical stability of aluminum. However, the fundamental intercalation processes and dynamics in these battery systems remain unresolved. Here, the energetics and dynamics of chloroaluminate ion intercalation in atomically thin single crystal graphite are investigated by fabricating mesoscopic devices for charge transport and optical microscopy. These mesoscopic measurements are compared to the high-performance rechargeable Al-based battery consisting of a few-layer graphene-multiwall carbon nanotube composite cathode. These composites exhibit a 60% capacity enhancement over pyrolytic graphite, while an ∼3-fold improvement in overall ion diffusivity is also obtained exhibiting ∼1% of those in atomically thin single crystals. Our results thus establish the distinction between intrinsic and ensemble electrochemical behavior in Al-based batteries and show that engineering ion transport in these devices can yet lead to vast improvements in battery performance.
基于氯铝酸盐电解质的可充电铝离子电池因铝的高丰度和化学稳定性而备受关注。然而，这些电池系统中的基本嵌入过程和动力学仍未得到解决。在此，通过制造用于电荷传输和光学显微镜的介观器件，研究了氯铝酸根离子在原子级薄的单晶石墨中的嵌入能量学和动力学。将这些介观测量结果与由几层石墨烯-多壁碳纳米管复合阴极组成的高性能可充电铝基电池进行了比较。这些复合材料的容量比热解石墨提高了60%，同时整体离子扩散率提高了约3倍，约为原子级薄单晶中的1%。因此，我们的结果确立了铝基电池中本征和整体电化学行为之间的区别，并表明在这些器件中设计离子传输仍可大幅提高电池性能。
