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iScience ll Article Figure 1. The reaction mechanism of CIB (A) Schematic representation of the rechargeable chloride ion battery. Herein, graphene, carbon black, and carbon nanotubes serve as cathode; Zn foil serves as cathode; and the saturated solutions of tetramethylammonium chloride was used as electrolyte. (B) The reaction mechanism of the negative electrode during the charging and discharging process. RESULTS AND DISCUSSION As we know, water molecule has strong solvation power with its highly polar and high dielectric constant that the cations (anion) are often limited in solvation shells formed by O (H) atoms (Cresce et al., 2015; Bu et al., 2019). When the tetramethylammonium chloride concentration is below 9.2 m, the solvation sheath of Cl consists of at least two layers (Figure 2A). The first layer is a chemical hydration layer, in which water molecules and ions are firmly combined; the second layer is a physical hydration layer, in which the attraction of water molecules and ions is relatively weak, and the first Cl solvation shell typically contains seven water molecules (Bouazizi et al., 2006). However, when salt concentration is above 11 m, there are not enough water molecules available to form the ‘‘classical’’ primary solvation sheath; thus the resultant ‘‘water-in-salt’’ solution can then be visualized as a liquefied salt. Figure 2B shows a comparison of the O-H stretching vibration and HOH bending vibration of water molecules in the different concentrated tetramethylammonium chloride electrolytes (Sun, 2009; Wu et al., 2017a; Frost et al., 2004). u2 and u3 represent the intensity of O-H stretching vibration and HOH bending vibration, respectively. It can be clearly seen that the O-H stretching vibration distinctly decreased with the consistence increase. The original shoulder at 3,248 cm1 gradually decreased, and the peak at 3,406 cm1 became the maximum at 25 m, showing that the strong hydrogen bonds of free water molecules were significantly destroyed. In addition, the ratio of u3 to u2 increased as the concen- tration increased, indicating that the destructive effect on the hydrogen bonds between water mole- cules is gradually increased as the concentration increases. The destruction of the hydrogen bonds re- duces the activity of free water molecules, and hydrogen evolution reaction is not easy to occur during charging and discharging. OPEN ACCESS iScience 24, 101976, January 22, 2021 3PDF Image | aqueous chlorine ion battery
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