Abstract

The high energy density and long cycling life of zinc-based batteries are restricted by the single electrochemical reaction system. To improve the electrochemical performance of batteries, electrode materials, electrolytes and membranes are regularly modified, while the construction of battery systems is often neglected. Herein, a multifunctional electrode was prepared via 3D printing, which successfully coupled the metal oxide/hydroxide-zinc battery (MZB) reaction and rechargeable zinc-air battery (RZAB) reaction. The ultrathick hierarchical 3D electrode provided a tunable capacity for the MZB system, which enabled the possibility for feasible output regulation of this hybrid system. The active material NiCoLDH was discovered to undergo structure reconstruction during cycling, which revealed the capacity fading mechanism. The delicate system design and discovery ensured a high-performance battery configuration and revealed the corresponding mechanism, opening a new avenue for developing high-performance zinc batteries.

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