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ARTICLE NATURE COMMUNICATIONS | https://doi.org/10.1038/s41467-020-20334-6 dendrite formed within 900 s at 80 mA cm−2 (Supplementary Fig. 32 and Supplementary Movie 20). Comparing with the pristine Zn electrode, which starts to show dendrite formation after just 100s (Supplementary Fig. 27 and Supplementary Movie 2), the flat Zn-Mn alloy shows the good capability to control the surface reaction and suppress the dendrite formation. On the other hand, the 3D Zn-Mn alloy does not show obvious dendrite formation after 8200 s of Zn deposition (Supplementary Fig. 33 and Supplementary Movie 9–13) under the same experimental conditions. Besides, we have fabricated a 3D Zn substrate without Mn, and the result shows improved perfor- mance comparing with the pristine Zn surface but still out- performed by the 3D Zn-Mn alloy (Supplementary Fig. 22). These results indicate that by coupling with the Zn-Mn alloy composition, the 3D nanostructures help to control the deposi- tion kinetics and further minimized the dendrite growth. Electrochemical performance of Zn-Mn anode in aqueous Zn batteries. To demonstrate the practical performance of the Zn- Mn anode in aqueous batteries, we assembled ZABs using com- mercial Pt/C@RuO2 as the cathode and Zn-Mn alloy as the anode (Supplementary Fig. 34a). A control battery was assembled using the pristine Zn as the anode for a comparison. The ZABs using Zn-Mn anodes showed excellent charge/discharge cycling stabi- lity for over 6000min test without degradation at a current density of 10 mA cm−2. In contrast, the ZABs using Zn anodes failed quickly after 2760 min test with a huge hysteresis (Fig. 4a). The galvanostatic discharge capacities of ZABs using different anodes were recorded (Fig. 4b and Supplementary Fig. 34b). Note that ZABs (Zn3Mn) and ZABs (Zn) are used to represent the batteries using Zn3Mn and Zn anodes, respectively, to reduce the wordy description. At a high current density of 30 mA cm−2, the ZABs (Zn3Mn) delivered an extremely high discharge capa- city of 816.3 mAh gZn−1 corresponding to an energy density of 798.3WhkgZn−1, higher than those of ZABs (Zn; 784mAh gZn−1 and 657 Wh kgZn−1) and superior to the recent bench- marking ZABs49–51. The significantly improved performance of the ZABs (Zn3Mn) is ascribed to the sufficiently exposed active areas in the hierarchically porous 3D architectures via this sur- face/interface engineering52. To further demonstrate the out- standing ZABs (Zn3Mn) performance, we used our most recently developed materials composed of the co-incorporated platinum (Pt) and fluorine (F) in the PtCo nanosheets as a cathode to replace commercial Pt/C@RuO253. As a proof-of-concept, a high peak power density of 196 mW cm−2 (Fig. 4c) was achieved by ZABs (Zn3Mn), which was much higher than that of ZABs (Zn) (130 mW cm−2). Besides, the Zn-Mn alloy is also mechanically robust and can be used for flexible ZABs. The flexible ZABs (Zn3Mn) in tandem cells exhibited nearly doubled voltages under different current densities. Under repeated twisting, the flexible tandem ZABs (Zn3Mn) retained a stable voltage and sustained an electric fan without any malfunction (Fig. 4d and Supplementary Movie 21). At the same time, the voltages of tandem ZABs (Zn3Mn) at high current densities were quite stable, confirming the outstanding performance for the Zn-Mn anode (Supple- mentary Fig. 35). Moreover, we assembled ZIBs full cells using MnO2 cathodes, Zn-Mn alloy anodes, and seawater-based elec- trolyte (2 M ZnSO4 and 0.1 M MnSO4 in seawater) to evaluate the electrochemical performance of Zn-Mn anode for aqueous ZIBs (Supplementary Fig. 36). The addition of Mn2+ in the electrolytes would improve the reversibility, greatly enhance the utilization of MnO2 active material, and suppress the dissolution of MnO2 in aqueous Zn//MnO2 batteries2,54. The ZIBs (Zn3Mn) using seawater-based electrolytes presented a higher capacity (373.2 mAh g−1, Fig. 4e) at 0.5 C and higher discharge voltage plateaus than that of ZIBs (Zn) (262.5 mAh g−1), confirming a more efficient charge transfer dynamics based on the Zn-Mn anode. We also investigated the anti-interference property of Zn-Mn anode against hetero-ions such as Na+ and Mg2+ in the seawater- based electrolyte. As a control experiment, the ZIBs (Zn3Mn) using Na+-containing electrolyte (2M Na2SO4 in seawater) showed a noticeable capacity of 30 mAh g−1, indicating a considerable storage capability in the ZIBs (Zn3Mn; Supplemen- tary Fig. 37). Besides, we used a Mg2+-containing electrolyte (2 M MgSO4 in seawater) to test the Mg2+ anti-interference property in the ZIBs (Zn3Mn). A distinct intercalation behavior was observed in the ZIBs (Zn3Mn) with a high initial capacity of 110 mAh g−1 (Supplementary Figs. 38 and 39a, b) compared with the pristine Zn anode (Supplementary Fig. 40). We also investigate the impact of hetero-ions (Na+ and Mg2+) on the electro- chemical performance of Zn-Mn alloy in the symmetric Zn-Mn// Zn-Mn cells (Supplementary Fig. 39c, d). And the anti- interference property of Zn-Mn anode against the other hetero- ions, including Ca2+ and Cl−, has also been investigated as shown in Supplementary Fig. 41, confirming the insignificant effect of hetero-ions (e.g., Ca2+ and Cl−) on the electrochemical performance of Zn-Mn alloy. The results also confirmed the highly anti-interference behaviors of the Zn-Mn anode. Further- more, the ZIBs (Zn3Mn) using seawater-based electrolyte exhibited a stable capacity of 300 mAh g−1 at 1 C, whereas the ZIBs (Zn) delivered a much lower capacity of 130mAh g−1 (Fig. 4f), demonstrating the superior electrochemical performance of ZIBs based on Zn-Mn anode in the seawater-based electrolyte. In particular, the self-discharge test of ZIBs (Zn3Mn) using the seawater-based electrolyte showed no drop in open-circuit voltage for 120 h (Supplementary Fig. 42). Furthermore, at a high rate of 4 C (Fig. 4g), the ZIBs (Zn) failed quickly after 368 cycles due to dendrite growth and short-circuit. In sharp contrast, the ZIBs (Zn3Mn) could keep a very stable performance over 2000 cycles without any dendrite growth and short-circuit (Supplementary Fig. 43), suggesting outstanding stability under harsh conditions far surpassing those of other benchmarking Zn anodes (Supple- mentary Table 3). The slow activation of the Zn//MnO2 batteries as shown in Fig. 4g could be caused by: (i) the diffusing paths of Zn2+ ion are gradually constructed due to the continuous infiltration of electrolytes after cycling; (ii) during the electrode activation process, more reactive sites could be exposed and the ionically conductive network of Zn2+ ion is greatly improved at the electrolyte/electrode interface55,56. To further demonstrate the broader impacts of the proposed concept in the battery field, we electrodeposited 3D Zn-Cu alloy (Supplementary Fig. 44), which could be another materials for high-performance aqueous batteries. Note that the 3D Zn-Cu anode is identified here as a potential extension of the proposed strategy for anode stabiliza- tion. We will fully discuss the battery performance of the Zn-Cu anode in our future work. To understand the reaction mechanism and confirm the structural changes of the electrodes during the charge/discharge processes for ZIBs (Zn3Mn), we performed ex-situ X-ray absorption spectroscopy (XAS) measurements53,57,58 on the Zn- Mn anodes and MnO2 cathodes at pristine, fully charged, and fully discharged states. For MnO2 cathodes, we tested the intercalation behaviors of Zn-Mn/MnO2, which existed in the seawater-based electrolyte, by using the Mg2+-containing elec- trolyte. X-ray absorption near edge structure (XANES, Supple- mentary Fig. 45) on MnO2 cathode shows distinct edge shifts. At the fully discharged state for MnO2 cathode, the XANES spectrum at Mn K-edge moves to the lower energy compared to that of the pristine MnO2 cathode, suggesting the lower oxidation state of Mn and the successful intercalation of hetero- ions in the bulk structure. Furthermore, XANES of charged 8 NATURE COMMUNICATIONS | (2021)12:237 | https://doi.org/10.1038/s41467-020-20334-6 | www.nature.com/naturecommunicationsPDF Image | high-performance dendrite-free seawater-based batteries
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