High-Capacity Rechargeable Li/Cl2Batteries with Graphite Positive Electrodes

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

Research output: Contribution to journalArticlepeer-review

20 Scopus citations

Abstract

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-1reversible 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 Cl2for reversible NaCl/Cl2or LiCl/Cl2redox 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/Cl2battery, attaining high battery performance after activation in carbon dioxide (CO2) at 1000 °C (DGr_ac) with the first discharge capacity ∼1910 mAh g-1and 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/Cl2redox. This work opens up widely available, low-cost graphitic materials for high-capacity alkali metal/Cl2batteries. Lastly, we employed mass spectrometry to probe the Cl2trapped in the graphitic positive electrode, shedding light into the Li/Cl2battery operation.

Original languageEnglish
Pages (from-to)22505-22513
Number of pages9
JournalJournal of the American Chemical Society
Volume144
Issue number49
DOIs
StatePublished - 14 Dec 2022

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