材料科学
吡嗪
阴极
锂(药物)
氧化还原
纳米技术
醌
溶解
二胺
分子
组合化学
化学工程
电化学
电极
有机化学
高分子化学
冶金
内分泌学
工程类
物理化学
化学
医学
作者
Peng Zhang,Xiaotang Gan,Liang Huang,Junxiao Wang,Minle Li,Zijun Hu,Rui Wang,Tingting Yu,Zhiping Song
标识
DOI:10.1021/acsami.4c00586
摘要
Organic cathode materials (OCMs) have tremendous potential to construct sustainable and highly efficient batteries beyond conventional Li-ion batteries. Thereinto, quinone/pyrazine hybrids show significant advantages in material availability, energy density, and cycling stability. Herein, we propose a facile method to synthesize quinone/pyrazine hybrids, i.e., the condensation reaction between ortho-diamine and bromoacetyl groups. Based on it, we have successfully synthesized three 1,4-diazaanthraquinone (DAAQ) dimers, including 2,2′-bi(1,4-diazaanthraquinone) (BDAAQ) with an exceptional theoretical capacity of 512 mAh g–1 based on the eight-electron reaction. It can be fully utilized in Li batteries in a wide voltage range of 0.8–3.8 V, at the cost of inferior cycling stability. In an optimal voltage range of 1.4–3.8 V, BDAAQ exhibits one of the best comprehensive electrochemical performances for small-molecule OCMs, including a high specific capacity of 366 mAh g–1, an average discharge voltage of 2.26 V, as well as a respectable capacity retention of 59% after 500 cycles. Moreover, the in-depth investigations reveal the redox reaction mechanisms based on C═O and C═N groups as well as the capacity fading mechanisms based on dissolution–redeposition behaviors. In brief, this work provides an instructive synthesis method and mechanism understanding of high-performance OCMs based on a quinone/pyrazine hybrid structure.
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