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iScience ll Article OPEN ACCESS Figure 3. Electrochemical performance of chlorine-ion battery with different electrodes in the saturated solutions of tetramethylammonium chloride Typical charge-discharge voltage profiles at 1 A g1 between 0.8 and 2.6 V of (A) carbon black/graphite, (B) carbon black/Zn, (C) carbon nanotube/Zn, and (D) graphene/Zn electrodes in the fifth cycle. Cycle life diagram of (E) carbon black/graphite, (F) carbon black/Zn, (G) carbon nanotube/Zn, and (H) graphene/Zn electrode. CH3 experiences a shift from 3,027 cm1 to 3,043 cm1 with the increasing concentration from 1 to 25 m, and the width of this band became narrow. This change can be attributed to the transition from ion pairs separated from water to contact ion pairs of Cl and (CH3)4N+ ions and the increasing order of electrolyte structure. This orderly electrolyte structure should inhibit the movement of water molecules, resulting in the reduced activity of free water molecules. The electrochemical stability window for these aqueous electrolytes was evaluated with linear sweep voltammetry (LSV) on graphite foil electrodes, whose scans are shown in Figure 2D. The overall stability win- dow extends with the increasing concentration of the ClN(CH3)4 electrolyte, with both hydrogen and oxy- gen deposition potentials far beyond the thermodynamic stability limits of water. Specifically, the electro- chemical stability window for the 1 m ClN(CH3)4 electrolyte was 2.20 V (from 1.15 to 1.05 V versus SCE) and the electrochemical stability window for the 25 m ClN(CH3)4 WIS electrolyte was 3.10 V (from 1.8 to 1.3 V versus SCE), showing a 0.9 V expansion of the electrochemical stability window. The electrochemical performances of CIBs with different electrodes were investigated in assembled soft pack battery. Figure 3A shows the charge-discharge curves of the battery using carbon black as cathode and graphite foil as anode. The battery delivers a discharge capacity of 70 mAh g1 (cut off 0.5V) and the open-circuit voltage at around 2.6 V. A discharged capacity of 46 mAh g1 was observed after 300 charge-discharge cycles, with a capacity retention of 65.7% (Figure 3E). Such an extraordinary high-voltage feature can be attributed to the fact that the chlorine-water-in-salt electrolyte offers a 3.1 V window through suppressing hydrogen evolution on anode and reducing the overall electrochemical activity of water on cathode, providing a high-voltage feature. Furthermore, it is feasible to explore a suitable anode material to improve the electrochemical perfor- mance of this battery. When zinc is used as anode, the electrochemical performance of battery with different cathode materials is shown in Figures 3B–3D and 3F–3H. As shown in Figures 3B and 3F, when carbon black was used as cathode, the reversible discharge capacity was 102 mAh g1, and the discharge platforms were about 2.6 V and 2.1V. And the battery delivered a discharge capacity of 45 mAh g1 in the first cycle with a gradual rise in capacity in the first few cycles, reaching the maximum value of 102 mAh g1 at the 60th discharge followed by stable cycling afterward. The increase in capacity for the initial sixty cycles can be related to the activation of the electrodes. A discharged capacity of 72.4 mAh g1 was observed iScience 24, 101976, January 22, 2021 5PDF Image | aqueous chlorine ion battery
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