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density of 0.947 FSI‐ anions per nm2 of nitrogen‐accessible surface at 120 mA g‐1. Having the highest specific surface area and largest micropore volume, ZTC was selected, as expected, for all further detailed electrochemical analyses. Upon extended electrochemical cycling, it was observed that reversible operation (coulombic efficiency of >99%) of ZTC as the cathode in a KFSI DIB was achieved after the first six cycles (see Figure S11) and could be maintained for sev‐ eral hundred cycles (Figure 3b). At 120 mA g‐1, the stable dis‐ charge capacity was increased slightly up to 141 mAh g‐1 after >300 cycles. The dependence of the specific discharge capac‐ ity and average discharge voltage on current density were de‐ termined by variable current cycling as shown in Figures 3c‐ 3d. At 480 mA g‐1, the stable discharge capacity was reduced to 97 mAh g‐1, ~70% of the initial stable discharge capacity at 120 mA g‐1. The charge/discharge voltage profiles at all cur‐ rent rates were found to be continuously sloped and do not exhibit any insertion/de‐insertion plateaux, which is consistent with the capacitive mechanism of charge storage as determined by cyclic voltammetry. At a current rate of 120 mA g‐1, the cathode‐specific energy and power density of ZTC are calculated to be 485 Wh kg‐1 and 418 W kg‐1, respectively, as detailed in the Supporting Infor‐ mation. The energy density was found to increase linearly with specific surface area while power density was approxi‐ mately constant across all of the porous carbon cathode ma‐ terials investigated (see Figure S16). Some scatter in the data is observed, indicating the likely relevance of other materials properties such as pore size, chemical composition, and edge contribution of the surface, as has been investigated in poly‐ aromatic hydrocarbon molecular solids25. On the other hand, the energy density of ZTC was found to decrease linearly with increasing current rate (modestly, as expected) while power density increased linearly with current rate (between 120‐ 1920 mA g‐1). ACS Applied Materials & Interfaces Page 10 of 17 Figure 3. Electrochemical Characterization of Microporous Carbon Materials as the Cathode in Dual‐Ion KFSI Batteries. (a) Galvanos‐ tatic charge/discharge voltage profiles of ZTC (black), and two lower surface area porous carbon materials (green and light green) during the 20th cycle, at a current rate of 120 mA g‐1. The capacity (at 2.65 V during discharge) is proportional to BET specific surface area (BET SA), related by a factor of 37.8 mAh per 1000 m2 of nitrogen‐accessible surface area. (b) Discharge capacity (open dia‐ monds) and coulombic efficiency (filled circles) over 300 cycles for ZTC KFSI DIBs cycled between 2.65‐4.7 V at 120 mA g‐1. (c) Galvanostatic charge/discharge voltage profiles of ZTC during the 12th, 17th, 22nd, 27th, and 32nd cycles, at various current rates be‐ tween 120‐1920 mA g‐1 as specified by color. (d) Discharge capacity retention (open diamonds) and coulombic efficiency (filled circles) over the same 50 cycles at the current rates indicated. 5 ACS Paragon Plus EnvironmentPDF Image | Zeolite-Templated Carbon as the Cathode
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