具有石墨正极的高容量可充电 Li/Cl2 电池,Journal of the American Chemical Society

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具有石墨正极的高容量可充电 Li/Cl2 电池
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-11-30 , DOI: 10.1021/jacs.2c07826
Guanzhou Zhu, Peng Liang, Cheng-Liang Huang, Cheng-Chia Huang, Yuan-Yao Li, Shu-Chi Wu, Jiachen Li, Feifei Wang, Xin Tian, Wei-Hsiang Huang, Shi-Kai Jiang, Wei-Hsuan Hung, Hui Chen, Meng-Chang Lin, Bing-Joe Hwang, Hongjie Dai

开发新型高容量和高能量密度的可充电电池对于未来几代消费电子产品、电动汽车和大规模储能应用具有重要意义。最近，我们报道了~3.5 V 钠/氯 (Na/Cl ₂ ) 和锂/氯 (Li/Cl ₂ ) 电池，其可逆容量高达 1200 mAh g ^–1，使用 Na 或 Li 金属作为负极, 无定形碳纳米球 (aCNS) 作为正极，氯化铝 (AlCl ₃ ) 溶解在亚硫酰氯 (SOCl ₂ ) 中，以氟化物为基础的添加剂作为电解质 [Zhu et al., Nature , 2021 , 596(7873), 525–530]。正极中 aCNS 的高表面积和大孔体积促进了 NaCl 或 LiCl 的沉积和 Cl ₂的捕获，用于可逆的 NaCl/Cl ₂或 LiCl/Cl ₂氧化还原反应和电池放电/充电循环。在这里，我们报道了一种最初低表面积/孔隙率的石墨 (DGr) 材料作为 Li/Cl ₂电池中的正极，在 1000 °C (DGr_ac) 的二氧化碳 (CO ₂ ) 中活化后获得了高电池性能首次放电容量 ∼1910 mAh g ^–1，循环容量高达 1200 mAh g ^–1. 非原位拉曼光谱和 X 射线衍射 (XRD) 揭示了石墨在电池循环过程中的演变，包括嵌入/脱嵌和剥离，从而产生足够的孔隙来容纳 LiCl/Cl ₂氧化还原。_{这项工作为高容量碱金属/Cl 2}电池开辟了广泛可用的低成本石墨材料。最后，我们采用质谱法探测捕获在石墨正极中的 Cl _{2 ，为 Li/Cl}₂电池的运行提供了线索。

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High-Capacity Rechargeable Li/Cl2 Batteries with Graphite Positive Electrodes

Developing new types of high-capacity and high-energy density rechargeable batteries is important to future generations of consumer electronics, electric vehicles, and mass energy storage applications. Recently, we reported ∼3.5 V sodium/chlorine (Na/Cl₂) and lithium/chlorine (Li/Cl₂) batteries with up to 1200 mAh g^–1 reversible capacity, using either a Na or a Li metal as the negative electrode, an amorphous carbon nanosphere (aCNS) as the positive electrode, and aluminum chloride (AlCl₃) dissolved in thionyl chloride (SOCl₂) with fluoride-based additives as the electrolyte [Zhu et al., Nature, 2021, 596 (7873), 525–530]. The high surface area and large pore volume of aCNS in the positive electrode facilitated NaCl or LiCl deposition and trapping of Cl₂ for reversible NaCl/Cl₂ or LiCl/Cl₂ redox reactions and battery discharge/charge cycling. Here, we report an initially low surface area/porosity graphite (DGr) material as the positive electrode in a Li/Cl₂ battery, attaining high battery performance after activation in carbon dioxide (CO₂) at 1000 °C (DGr_ac) with the first discharge capacity ∼1910 mAh g^–1 and a cycling capacity up to 1200 mAh g^–1. Ex situ Raman spectroscopy and X-ray diffraction (XRD) revealed the evolution of graphite over battery cycling, including intercalation/deintercalation and exfoliation that generated sufficient pores for hosting LiCl/Cl₂ redox. This work opens up widely available, low-cost graphitic materials for high-capacity alkali metal/Cl₂ batteries. Lastly, we employed mass spectrometry to probe the Cl₂ trapped in the graphitic positive electrode, shedding light into the Li/Cl₂ battery operation.

更新日期：2022-11-30

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