Asymmetric Electrode Design for High-Area Capacity and High-Energy Efficiency Hybrid Zn Batteries.

Abstract

Compared to Zn-air batteries, by integrating Zn-transition metal compound reactions and oxygen redox reactions at the cell level, hybrid Zn batteries are proposed to achieve higher energy density and energy efficiency. However, attaining relatively higher energy efficiency relies on controlling the discharge capacity. At high area capacities, the proportion of the high voltage section can be neglected, resulting in a lower energy efficiency similar to that of Zn-air batteries. Here, a high-loading integrated electrode with an asymmetric structure and asymmetric wettability is fabricated, which consists of a thick nickel hydroxide (Ni(OH)2) electrode layer with vertical array channels achieving high capacity and high utilization, and a thin NiCo2O4 nanopartical-decorated N-doped graphene nanosheets (NiCo2O4/N-G)catalyst layer with superior oxygen catalytic activity. The asymmetric wettability satisfies the wettability requirements for both Zn-Ni and Zn-air reactions. The hybrid Zn battery with the integrated electrode exhibits a remarkable peak power density of 141.9mWcm-2, superior rate performance with an energy efficiency of 71.4% even at 20mAcm-2, and exceptional cycling stability maintaining a stable energy efficiency of ≈84% at 2mAcm-2 over 100 cycles (400 h).