Raising the redox potential in carboxyphenolate-based positive organic materials via cation substitution.
Raising the redox potential in carboxyphenolate-based positive organic materials via cation substitution.
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DOI：
10.1038/s41467-018-06708-x
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发表时间：
2018-10-23
影响因子：
16.6
通讯作者：
Poizot P
中科院分区：
文献类型：
--
作者：
Jouhara A;Dupré N;Gaillot AC;Guyomard D;Dolhem F;Poizot P
满足对电存储设备不断增长的需求需要上级和“绿色”电池技术。在导电聚合物发现近40年后，锂有机电池的长期循环稳定性现已实现。然而，高电压锂化有机阴极材料的合成相当具有挑战性，因此目前存在非常少的全有机锂离子电池的实例。本文中，我们提出了导致锂化有机电极材料的氧化还原电位显著增加的发明性化学方法。这是通过调节氧化还原活性有机骨架中的电子效应来实现的，这是由于在主体结构中永久存在的旁观者阳离子表现出高离子电位（或电负性）。因此，用（2，5-氧代）对苯二甲酸镁代替（2，5-氧代）对苯二甲酸锂能够实现接近+800 mV的电压增益。该化合物还能够通过羧酸酯官能团充当负电极，展示了显示2.5V输出电压的全有机对称锂离子电池。有机电极材料可以实现新一代电池所需的新奇化学。在这里，作者显示了Mg（Li 2）-p-DHT作为锂化阴极材料的合成和电化学性能，由于主体结构中存在旁观者阳离子，该锂化阴极材料在3.4 V下循环。
Meeting the ever-growing demand for electrical storage devices requires both superior and “greener” battery technologies. Nearly 40 years after the discovery of conductive polymers, long cycling stability in lithium organic batteries has now been achieved. However, the synthesis of high-voltage lithiated organic cathode materials is rather challenging, so very few examples of all-organic lithium-ion cells currently exist. Herein, we present an inventive chemical approach leading to a significant increase of the redox potential of lithiated organic electrode materials. This is achieved by tuning the electronic effects in the redox-active organic skeleton thanks to the permanent presence of a spectator cation in the host structure exhibiting a high ionic potential (or electronegativity). Thus, substituting magnesium (2,5-dilithium-oxy)-terephthalate for lithium (2,5-dilithium-oxy)-terephthalate enables a voltage gain of nearly +800 mV. This compound being also able to act as negative electrode via the carboxylate functional groups, an all-organic symmetric lithium-ion cell exhibiting an output voltage of 2.5 V is demonstrated. Organic electrode materials could enable novelty chemistry required by the new generation of batteries. Here the authors show the synthesis and electrochemical performance of Mg(Li2)-p-DHT as a lithiated cathode material that cycles at 3.4 V due to the presence of a spectator cation in the host structure.
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影响因子：
23.5
作者：
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通讯作者：
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