共轭体系
杂原子
材料科学
阴极
聚合
有机自由基电池
轨道能级差
光化学
咔唑
醌
电子转移
聚合物
离域电子
电化学
化学
有机化学
电极
物理化学
分子
戒指(化学)
作者
Xin Shi,Ang Yi,Qiyu Liu,Yan Zhang,Shiwei Lin,Xihong Lu
出处
期刊:ACS Nano
[American Chemical Society]
日期:2023-12-06
卷期号:17 (24): 25005-25013
被引量:3
标识
DOI:10.1021/acsnano.3c07346
摘要
π-conjugated organic compounds with a good charge transfer ability and rich redox functional groups are promising cathode candidates for air-rechargeable aqueous Zn-based batteries (AAZBs). However, the output voltage of even the state-of-the-art π-conjugated organic cathodes lies well below 0.8 V, resulting in insufficient energy density. Herein, we design a nonplanar π-conjugated sulfur heterocyclic quinone polymer (SHQP) as an advanced cathode material for AAZBs by polymerization 1,4-Benzoquinone (BQ) and S heteroatoms periodically. The extended π-conjugated plane and enhanced aromaticity endow SHQP with a more sensitive charge transfer ability and robust structure. Furthermore, the delocalized π electrons in the whole system are insufficient as the π orbit of the S heteroatom is not in the same plane with the π orbit of BQ due to its folded configuration, resulting in negligible variation of electron density around C═O after the polymerization. Thus, the output voltage of SHQP shows no significant decrease even though the thioether bond (-S-) functions as electron donor. Consequently, the Zn/SHQP AAZBs can deliver a record high midpoint discharging voltage (0.95 V), rate performance (119 mAh g-1 at 10 A g-1), and durability (98.7% capacity retention after 200 cycles) across a wide temperature range.
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