电化学制备氢氧化钴/氢氧化氧混合相作为锌离子电池正极

Fuwei Li, Yunbo Zhu, Hiroshi Ueno, Ting Deng
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摘要

氢氧化钴是一种被广泛研究的超级电容器和碱性锌离子电池电极材料。Co(OH)2的大层间距也有利于Zn离子的储存。然而,由于Co(OH)2的两性性质,它在酸性ZnSO4电解质中非常不稳定。本文采用两步电化学法制备了Co(OH)2/CoOOH混合相。作为水性锌离子电池(AZIB)的正极材料,Co(OH)2/CoOOH在0.05 a g−1时的最大容量为164 mAh g−1,能量密度为275 Wh kg−1。由于具有较低的电荷转移电阻,在1.6 a g−1时可保持87 mAh g−1的容量,表现出良好的混合相速率性能。基于密度泛函理论(DFT)的各种光谱分析和模拟表明,混合相的热稳定性比纯Co(OH)2高,因为其局部结构无序性较小。减少的Co-Co和Co-O壳层增加了混合相的机械强度,以容纳Zn2+离子并承受静电排斥,从而增强了循环稳定性。混合相在0.05 a g−1的电流密度下也具有良好的稳定性。经过200次循环后,容量保留率为78%,库仑效率很高。这些结果为制备高性能锌离子电池用LDH提供了一条新途径。
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An Electrochemically Prepared Mixed Phase of Cobalt Hydroxide/Oxyhydroxide as a Cathode for Aqueous Zinc Ion Batteries
Cobalt hydroxide is a widely studied electrode material for supercapacitor and alkaline zinc ion batteries. The large interlayer spacing of Co(OH)2 is also attractive to store Zn ions. However, Co(OH)2 is quite unstable in the acidic ZnSO4 electrolyte due to its amphoteric nature. Herein, we synthesized a mixed phase of Co(OH)2/CoOOH via a two-step electrochemical preparation. As the cathode material for an aqueous zinc ion battery (AZIB), Co(OH)2/CoOOH delivered a maximum capacity of 164 mAh g−1 at 0.05 A g−1 and a high energy density of 275 Wh kg−1. Benefiting from the low charge-transfer resistance, a capacity of 87 mAh g−1 was maintained at 1.6 A g−1, showing a good rate performance of the mixed phase. Various spectroscopy analyses and simulations based on the density functional theory (DFT) suggested a higher thermal stability of the mixed phase than pure Co(OH)2, due to its less local structural disorder. The reduced Co-Co and Co-O shells increased the mechanical strength of the mixed phase to accommodate Zn2+ ions and endure the electrostatic repulsion, resulting in an enhanced cycling stability. The mixed phased also delivered a good stability at the current density of 0.05 A g−1. After 200 cycles, a capacity retention of 78% was retained, with high Coulombic efficiencies. These results provide a new route to synthesize high-performance LDH for aqueous zinc ion batteries.
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