Function-oriented design of conjugated carbonyl compound electrodes for high energy lithium batteries
Function-oriented design of conjugated carbonyl compound electrodes for high energy lithium batteries
复制标题
高能锂电池共轭羰基化合物电极的功能导向设计
DOI：
10.1039/c3sc22093a
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发表时间：
2013-01-01
期刊：
影响因子：
8.4
通讯作者：
Chen, Jun
中科院分区：
文献类型：
--
作者：
Liang, Yanliang;Zhang, Peng;Chen, Jun
有机羰基化合物是潜在的低成本、可持续和高能量密度的电极材料，但在电池应用中受到不令人满意的活性位点利用率、低放电电势和低速率放电-充电性能的困扰。本文公开了具有多电子反应的羰基化合物作为可再充电锂电池的正极材料的面向功能的设计，表明分子轨道分布和能量学可用于预测羰基利用率和调节氧化还原电位。通过在扩展的共轭体系中嵌入前芳族1，2-二羰基部分，所需的分子整合了所有已知的稳定因子，并能够完全吸收四锂。值得注意的是，两种新的羰基电极，芘-4，5，9，10-四酮和1，10-菲咯啉-5，6-二酮，分别提供了360 mA h g（-1）的可逆容量和2.74 V的平均工作电位，为设计用于高效能量存储和转换的锂电池的高能有机正极提供了见解。
Organic carbonyl compounds are potentially low-cost, sustainable, and high energy density electrode materials, but are plagued by unsatisfactory active-site utilization, low discharge potentials and low rate discharge-charge performance in battery applications. We herein disclose a function-oriented design of carbonyl compounds with multi-electron reactions as positive electrode materials for rechargeable lithium batteries, showing that molecular orbital profiles and energetics can be applied for the prediction of carbonyl utilization and modulation of redox potentials. By embedding pre-aromatic 1,2-dicarbonyl moieties in the extended conjugated systems, the desirable molecules integrate all known stabilizing factors and enable full four-Li uptake. Remarkably, two new carbonyl electrodes, pyrene-4,5,9,10-tetraone and 1,10-phenanthroline-5,6-dione, deliver a reversible capacity of 360 mA h g(-1) and an average working potential of 2.74 V, respectively, providing insights in designing high-energy organic positive electrodes of lithium batteries for efficient energy storage and conversion.