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Aqueous zinc-ion batteries (ZIBs) have significant potential for large energy storage systems because of their high energy density, cost-effectiveness and environmental friendliness. However, the limited voltage window, poor reaction kinetics and structural instability of cathode materials are current bottlenecks which contain the further development of ZIBs. In this work, we rationally design a Ni-doped V2O5@3D Ni core/shell composite on a carbon cloth electrode (Ni-V2O5@3D Ni@CC) by growing Ni-V2O5 on free-standing 3D Ni metal nanonets for high-voltage and high-capacity ZIBs. Impressively, embedded Ni doping increases the interlayer spacing of V2O5, extending the working voltage and improving the zinc-ion (Zn302+) reaction kinetics of the cathode materials; at the same time, the 3D structure, with its high specific surface area and superior electronic conductivity, aids in fast Zn302+ transport. Consequently, the as-designed Ni-V2O5@3D Ni@CC cathodes can operate within a wide voltage window from 0.3 to 1.8 V vs. Zn30/Zn302+ and deliver a high capacity of 270 mAh g−1 (~1050 mAh cm−3) at a high current density of 0.8 A g−1. In addition, reversible Zn2+ (de)incorporation reaction mechanisms in the Ni-V2O5@3D Ni@CC cathodes are investigated through multiple characterization methods (SEM, TEM, XRD, XPS, etc.). As a result, we achieved significant progress toward practical applications of ZIBs. [ABSTRACT FROM AUTHOR] more...

The demand for high‐energy‐density and safe energy storage devices has spurred increasing interest in high‐voltage rechargeable magnesium batteries (RMB). As electrolytes are the bridge connecting the cathode and anode materials, the development of high‐voltage electrolytes is the key factor in realizing high‐voltage RMBs. This concept presents an overview of three chloride‐free electrolyte systems with wide electrochemical windows, together with the degradation mechanisms and modification strategies at the anode/electrolyte interphase. Finally, future directions in stabilizing Mg anodes and realizing high‐voltage RMBs are highlighted. [ABSTRACT FROM AUTHOR] more...