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Batteries 2022, 8, 181 5 of 13 Batteries 2022, 8, 181 enlargement of the resultant aggregation sizes (EDS mapping of Mn element in the cross‐ section of the 6.0 g/L electrode, see Figure 2e). Hence, during the gradual stacking of the solid component on the current collector (Figure S2d–f), the enlarged aggregations lead to the formation of the vacant areas between them from the bottom to the top of the electrode (see Figure 2e) due to the heterogeneous interlocking of the deposited product (Figure 2f,g), leading to the construction of free pathway networks for electrolyte penetration and 5 of 12 surface area to accommodate violent structural deformation of the electrode induced by an adequate surface area to accommodate violent structural deformation of the electrode the electrochemical reactions of the Na ions [45]. induced by the electrochemical reactions of the Na ions [45]. Figure 1. (a–d) Surface‐view and (e–h) cross‐section SEM images of the Na0.44MnO2 electrodes with Figure 1. (a–d) Surface-view and (e–h) cross-section SEM images of the Na0.44MnO2 electrodes with increasing solution concentrations from 0.5 to 8.0 g/L fabricated by the one‐pot spraying process, (i) increasing solution concentrations from 0.5 to 8.0 g/L fabricated by the one-pot spraying process, comparison of the electrode factors (loading mass (black histogram), packing density (blue histo‐ (i) comparison of the electrode factors (loading mass (black histogram), packing density (blue his- gram), thickness, aggregation size, and pore size) with the varying solution concentrations, and (j) togtrhaemX)R,Dthcicukrvnessosf,alglgthregealetcitornodseisz.e,andporesize)withthevaryingsolutionconcentrations,and (j) the XRD curves of all the electrodes. The galvanostatic charge/discharge voltage profiles measured at 0.1 C expose a dif- ference in the electrochemical behavior among the electrodes (Figure 3a). Compared to the dense electrode structure made by the suspension concentration of 0.5 g/L, the charge/discharge profiles of the electrodes made by the higher suspension concentrations show six more distinct plateaus, indicating the consecutive phase transitions of Na0.44MnO2 during Na-ion intercalation and deintercalation [46], especially for the electrode made by the suspension concentration of 6.0 g/L, resulting in the maximum of the initial discharge capacity (121.6 mAh/g). This is attributed to the open channels within the electrode pro- viding an effective surface area for the electrochemical reactions of the Na ions with the Na0.44MnO2 active material [32]. Furthermore, as shown in Figure 3b,d, while the 0.5 g/L electrode shows rapid degradation of the specific capacity at the accelerated current densi- ties from 0.1 to 10 C, the 6.0 g/L electrode exhibited superior capacity value and capacity retention at increasing C rates to 10 C. The 6.0 g/L electrode also exhibited higher volumet- ric capacities at 1 C and higher rates (Figure 3c), which can be attributed to the improvedPDF Image | Cathode Electrodes High-Rate Cycle-Stable Na-Ion Batteries
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