ZnAlxCo2–xO4 Spinels as Cathode Materials for Non-Aqueous Zn Batteries with an Open Circuit Voltage of ≤2 V,Chemistry of Materials

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ZnAlxCo2–xO4 Spinels as Cathode Materials for Non-Aqueous Zn Batteries with an Open Circuit Voltage of ≤2 V
Chemistry of Materials ( IF 7.2 ) Pub Date : 2017-11-03 00:00:00 , DOI: 10.1021/acs.chemmater.7b03340
Chengsi Pan ₁ , Ralph G. Nuzzo ₁ , Andrew A. Gewirth ₁

Affiliation

Rechargeable Zn batteries are promising energy storage alternatives for Li-ion batteries in part because of the high specific and volumetric capacities of Zn anodes, as well as their low cost, improved prospects for safety, and the fact that they are environmentally friendly. Development efforts, however, have focused mostly on aqueous electrolyte systems, which are intrinsically limited by the narrow electrochemical potential window of water. As a consequence, the use of alternative non-aqueous electrolytes has attracted a growing level of interest with the hope that they may provide higher operational voltages, which potentially could provide viable pathways to high-energy and high-power density Zn batteries. With regard to the latter, the considerable progress made in developing useful non-aqueous electrolyte chemistries for Zn anodes has not been matched by correlated progress regarding the development of useful cathode materials. In this work, a new series of spinels, ZnAl_xCo_2–xO₄, are reported and their utility as cathode materials for non-aqueous Zn-ion batteries is demonstrated. Full cells constructed using this new spinel as a cathode paired with a metal anode showed capacities over 100 cycles of 114 mAh/g and an onset potential of 1.95 V, which is the highest OCV yet reported for a non-aqueous Zn-ion battery system. The data show that the Zn²⁺ ions reversibly intercalate into the spinel structure during the charge–discharge processes, a compositional transformation directly correlated with a reversible conversion between Co⁴⁺ and Co³⁺ oxidation states within the lattice. The data illustrate that the Al³⁺-doped spinel structure is a robust candidate material for use in non-aqueous Zn batteries, suggesting guidelines for the design of more efficient multivalent cathode materials.

中文翻译：

ZnAl _x Co _{2– x} O ₄尖晶石作为开水电压≤2V的非水锌电池的阴极材料

可充电锌电池有望成为锂离子电池的储能替代品，部分原因是由于锌阳极的高比容量和体积容量，其成本低廉，安全性前景得到改善以及其对环境友好的事实。然而，开发工作主要集中在水性电解质体系上，其本质上受到水的狭窄电化学势能窗口的限制。结果，使用替代性非水电解质引起了越来越多的关注，希望它们可以提供更高的工作电压，这可能为高能量和高功率密度的Zn电池提供可行的途径。关于后者，在开发用于锌阳极的有用的非水电解质化学方面取得的重大进展还没有与在有用的阴极材料的开发方面的相关进展相匹配。在这项工作中，新的尖晶石系列ZnAl报道了_x Co_{2– x} O₄，并证明了它们作为非水Zn离子电池正极材料的用途。使用这种新型尖晶石作为阴极与金属阳极配对构成的全电池在100次循环中的容量为114 mAh / g，起始电位为1.95 V，这是非水Zn离子电池系统迄今报道的最高OCV。。数据表明，在充放电过程中，Zn²⁺离子可逆地插入到尖晶石结构中，其组成转变与晶格内Co⁴⁺和Co³⁺氧化态之间的可逆转化直接相关。数据表明，Al³⁺掺杂的尖晶石结构是用于非水Zn电池的可靠的候选材料，为设计更有效的多价阴极材料提供了指导。

更新日期：2017-11-05

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