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Zhao et al. (2014) BiCl3 Li OMIMCl-BMIMBF4 2.4V 3 181 Zhao et al. (2013) FeOCl Li PP14Cl- PP14TFSI 2.1V 30 132 Zhao et al. (2017) PPyCl@CNTs Li PP14Cl- PP15TFSI 2.2V 40 259 Gao et al. (2014) VOCl Mg PP14Cl-PC 1.95V 53 90 Gao et al. (2016) VOCl Li PP14Cl-PC 1.6V 100 184 Lakshmi et al. (2019) Sb4O5Cl2 Li PP14Cl-PC 1.5V 100 109 Yin et al. (2019) CoFe-Cl Li PP14Cl-PC 2V 100 280 Our work Graphene Zn C4H12ClN-H2O Carbon black Carbon nanotubes 2.6V 2,000 252 2.6V 1,000 194 2.6V 800 205 ll OPEN ACCESS Table 1. Comparison of our work with traditional CIBs Ref. Cathode Anode Electrolyte iScience Article Cycle Voltage life Energy density (Wh/kg) Energy density equal to the product of C and U, where C is capacity based on the total mass of cathode-active material, U is average discharge voltage. Rechargeable aqueous batteries are regarded as ideal choices for large-scale energy storage due to their high ionic conductivity, safety, low environmental impact, and low cost. However, the energy den- sity and output voltage of such batteries are limited by the narrow electrochemical stability window of water (1.23 V) (Kim et al., 2014; Luo et al., 2010; Pan et al., 2016). Therefore, expanding the electrochem- ical stability window of aqueous electrolytes is the key to the development of aqueous rechargeable batteries. Recently, water-in-salt electrolytes widened the electrochemical window of Li-ion battery to 3 V, which can deliver high cycling stability and excellent energy density (Suo et al., 2015). The wa- ter-in-salt concept has been applied to other types of aqueous electrochemical energy storage sys- tems, such as Na/Zn/K/Al-ion batteries and supercapacitors (Jiang et al., 2020; Zhao et al., 2016; Leo- nard et al., 2018; Zhou et al., 2019; Guo et al., 2019). The relatively lesser explored and overlooked area is the application of water-in-salt electrolytes for CIBs. Based on the abovementioned considerations, we first proposed carbon material (graphene, carbon nano- tubes, and carbon black) as cathode materials of CIBs and applied ‘‘water-in-salt’’ concept to widen the electrochemical window of chloride ion aqueous electrolytes. In this ‘‘water-in-salt’’ electrolyte system, the carbon cathode shows excellent cycling stability and electrochemical properties, and the discharge platform of battery is around 2.6V. Table 1 shows the comparison between our work and other represen- tative CIBs. It can be clearly seen that the cycle life of CIB has highly improved compared with the previous chloride ion batteries. When graphene is used as cathode material, especially, the cycle life of CIB can be up to 2000. This provides useful insight into the development of high-performance CIBs, which has been retarded by the issue of electrode dissolution in electrolyte. The electrochemical reaction mechanism of the battery was investigated in detail by Transmission Electron Microscope (TEM), infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and Raman spectra. The electrochemical reaction mechanism of the battery is based on the chloride ions shuttle via the ab- sorption/desorption reactions of C/Cn(Cl) at the cathode side. As shown in Figure 1A, during battery charge, the chloride ions desorb from metal anode and migrate to the carbon cathode. There, an ab- sorption reaction occurs, leading to the formation of Cn(Cl) phase (n is the molar ratio of carbon atoms to the absorbed Cl); during the discharging process, the chloride ions are desorbed from the carbon cathode and are captured by metal anode. For zinc anode (Figure 1B), during the battery discharge process, the chloride ions migrate to the zinc anode surface and the external electrons move from the anode to the cathode electrode in order to keep the balance of the internal circuit and external circuit. At the same time, the extranuclear electrons of zinc are pulled, but they have not completely separated from zinc, forming an intermediate state (Znd+) between Zn and Zn2+. At this time, there is an electrostatic attraction between the high concentration of chloride ions and the intermediate zinc, which makes the combination of chloride ions and Znd+ rely on weak intermolecular forces. During the battery charging progress, the electrons are reset, Znd+ becomes Zn, the electrostatic attraction disappears, and chloride ions desorb from the metal anode and migrate to the carbon cathode. 2 iScience 24, 101976, January 22, 2021PDF Image | aqueous chlorine ion battery
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