Highly durable organic electrode for sodium-ion batteries via a stabilized α-C radical intermediate.
Highly durable organic electrode for sodium-ion batteries via a stabilized α-C radical intermediate.
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DOI：
10.1038/ncomms13318
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发表时间：
2016-11-07
影响因子：
16.6
通讯作者：
Lu, Zhouguang
中科院分区：
文献类型：
--
作者：
Wu, Shaofei;Wang, Wenxi;Li, Minchan;Cao, Lujie;Lyu, Fucong;Yang, Mingyang;Wang, Zhenyu;Shi, Yang;Nan, Bo;Yu, Sicen;Sun, Zhifang;Liu, Yao;Lu, Zhouguang
制备具有长循环寿命和高容量的钠离子电池有机电极是一个挑战。由于不期望的副反应，钠化/脱钠过程中产生的高反应性自由基中间体可能是一个关键问题。在这里，我们展示了具有稳定的 α-C 自由基中间体的耐用电极。通过共振效应和空间效应，成功抑制了不成对电子的过度反应性，从而开发出循环稳定超过2000次且容量保持率为96.8%的电极。此外，α-自由基表现出三种状态之间的可逆转变：C=C； α-C·自由基；和α-C−阴离子。这种转变为电极提供了额外的 Na+ 存储，相当于每个 α-C 基团插入超过 0.83 个 Na+。中间自由基稳定策略对于设计具有增强循环寿命和储能能力的有机电极具有启发意义。 反应性自由基中间体可能是导致钠离子电池中有机电极快速降解的一个问题。在这里，作者展示了一种稳定的 α-C 自由基，它在 C=C、α-C 自由基和 α-C 阴离子状态之间表现出可逆转变，以促进长循环和提高容量。
It is a challenge to prepare organic electrodes for sodium-ion batteries with long cycle life and high capacity. The highly reactive radical intermediates generated during the sodiation/desodiation process could be a critical issue because of undesired side reactions. Here we present durable electrodes with a stabilized α-C radical intermediate. Through the resonance effect as well as steric effects, the excessive reactivity of the unpaired electron is successfully suppressed, thus developing an electrode with stable cycling for over 2,000 cycles with 96.8% capacity retention. In addition, the α-radical demonstrates reversible transformation between three states: C=C; α-C·radical; and α-C− anion. Such transformation provides additional Na+ storage equal to more than 0.83 Na+ insertion per α-C radical for the electrodes. The strategy of intermediate radical stabilization could be enlightening in the design of organic electrodes with enhanced cycling life and energy storage capability. Reactive radical intermediates can be a problem leading to fast degradation of organic electrodes in sodium-ion batteries. Here, the authors show a stabilized α-C radical displaying reversible transformations between C=C, α-C radical and α-C anionic states to facilitate long cycling and improved capacity.
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