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Nano-Micro Lett. (2022) 14:82 Page 7 of 13 82 (a) 10 8 6 4 2 00 (b) 120 90 60 30 25 20 15 116.9 μA 23.7 μA Zn (c)240 200 Initial state Steady state 200 240 Zn (d) 100 80 60 40 20 0 Zn (e) 0.2 0.0 −0.2 0.2 0.0 −0.2 2 4 Z′ (Ohm) 8 10 00 2.4 Ohm 17.0 μA Zeolite-Zn 13.5 μA 160 120 80 40 6 40 120 80 2.0 2.0 120 Z′ (Ohm) 0 2000 4000 6000 800010000 Time (s) 160 (f) Zn Zeolite-Zn Average CE: 93.9% Average CE: 99.1% 4.0 mAh cm-2 0 40 80 120 160 200 0 Cycle number 0.1 0.0 −0.1 2.5 mA cm-2 2.5 mAh cm-2 10% DOD 40 80 Time (h) 160 200 Zeolite-Zn 0.25 0.25 0.5 0.5 1.0 1.0 4.0 mA cm-2 Zeolite-Zn 0 50 100 150 200 250 300 350 400 450 500 Time (h) Fig. 2 a EIS plot of the zeolite layer. b Current–time (I-t) curves of a Zn||Zn and Zeolite-Zn||Zeolite-Zn symmetric cells stimulated by a con- stant polarization voltage of 10 mV. c EIS plot of the symmetric cells before (initial state) and after applying voltage polarization for 10,000 s (steady state). d Coulombic efficiencies (CEs) of a bare Zn||Cu and a Zeolite-Zn||Zeolite-Cu asymmetric cells in 1 M ZnSO4 electrolyte; the employed current density is 0.5 mA cm−2 with a striping upper-limit voltage of 0.5 V. e–f Voltage profiles of Zn||Zn and Zeolite-Zn||Zeolite-Zn symmetric cells during galvanostatic cycling test in 1 M ZnSO4 electrolyte S represents the layer thickness (66 μm) and area (2 cm2), respectively. It is worth noting that, the EIS-deduced ionic conductiv- ity is a total value contributed by all the charge carriers, including both cations and anions [54]. To determine the specific conductivity contribution by Zn2+, the transfer- ence numbers of Zn2+ (TZn2+) were tested by combin- ing potentiostatic polarization and EIS measurements (Fig. 2b–c) [48, 55]. In the potentiostatic polarization test, the bias voltage (ΔV = 10 mV) stimulates a large initial current (I0) at the beginning, which gradually decreases to a smaller steady-state current (Iss) due to the establish- ment of stable concentration polarization in the vicinity of the electrode. With the assistance of EIS-determined charge transfer impedances (R0, Rss, Fig. S8), the Zn2+ transference number (TZn2+) of the protecting layer can be calculated following Eq. (2) [56]: ΔV −R I0 = (2) Iss Compared to the Zn||Zn symmetric cell, the Zeolite- Zn||Zeolite-Zn cell is small in both I0 (23.7 vs. 116.9 μA) and Iss (13.5 vs. 17.0 μA, Fig. 2b), because of the suppression of anion-contributed ionic conductivity [54]. As a result, the TZn2+ of the symmetric cells is significantly improved from 0.15 to 0.53 by the zeolite layer. The simultaneous achieve- ment of high ionic conductivity and large Zn2+ transference number indicate that the zeolite layer is well-performed in both Zn2+-conducting and I3−-blocking [48]. In addition, the T0 2+ Zn ΔV −Rss 13 Voltage (V) Coulombic Efficiency (%) -Z′′ (Ohm) Voltage (V) Current (μA) -Z′′ (Ohm)PDF Image | Boosting Zn Battery by Coating a Zeolite‐Based Cation‐Exchange
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