Unveiled correlations between electron affinity and solvation in redox potential of quinone-based sodium-ion batteries
Unveiled correlations between electron affinity and solvation in redox potential of quinone-based sodium-ion batteries
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DOI：
10.1016/j.ensm.2019.01.017
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发表时间：
2019-05-01
影响因子：
20.4
通讯作者：
Jang, Seung Soon
中科院分区：
文献类型：
--
作者：
Kim, Ki Chul;Liu, Tianyuan;Jang, Seung Soon
采用第一性原理密度泛函理论方法，结合实验技术研究了7种醌衍生物的氧化还原性能和电荷存储性能，并评价了它们作为钠离子电池阴极的潜力。计算得到的氧化还原性质与其他性质，即电子亲和性（EA）、溶剂化能、电荷存储容量和能量密度全面相关。进一步验证了这种相关性不仅适用于醌类，也适用于其他有机分子。已建立的普遍相关性突出了三个主要结论。首先，EA和溶剂化能需要协同调整以达到特定的氧化还原电位。其次，蒽醌-2,6-二羧酸的优异性能可以用氧化还原电位与EA和溶剂化能的相关性来解释。第三，其他六种醌衍生物的计算值与实验值的差异主要是由Na结合构型造成的，突出表明亚稳Na结合情景显著增强了实验电荷容量。
First-principles density functional theory method is employed with experimental techniques to investigate the redox properties and charge storage performance of seven quinone derivatives and to assess their potential as cathodes in sodium-ion batteries. The computed redox properties are comprehensively correlated with other properties, namely, electron affinity (EA), solvation energy, charge storage capacity, and energy density. The correlations are further verified to be applied not only to quinones but also to other organic molecules. The established universal correlations highlight three main conclusions. First, EA and solvation energy need to be cooperatively tuned to achieve a specific redox potential. Second, the exceptionally high performance of anthraquinone-2,6-dicarboxylic acid can be explained by the correlation of the redox potential with EA and solvation energy. Third, the differences in the performance between the calculated and experimental values for the other six quinone derivatives mainly result from the Na binding configurations, highlighting the experimental charge capacity is extraordinarily enhanced by metastable Na binding scenarios.