A Pyrene-4,5,9,10-Tetraone-Based Covalent Organic Framework Delivers High Specific Capacity as a Li-Ion Positive Electrode.
A Pyrene-4,5,9,10-Tetraone-Based Covalent Organic Framework Delivers High Specific Capacity as a Li-Ion Positive Electrode.
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DOI：
10.1021/jacs.2c02196
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发表时间：
2022-06-01
影响因子：
15
通讯作者：
Cooper AI
中科院分区：
文献类型：
--
作者：
Gao H;Neale AR;Zhu Q;Bahri M;Wang X;Yang H;Xu Y;Clowes R;Browning ND;Little MA;Hardwick LJ;Cooper AI
具有电化学活性的共价有机骨架（COF）是一种很有前途的锂离子电池电极材料。然而，提高基于COF的电极的比容量需要具有增加的导电性和更高浓度的氧化还原活性基团的材料。在这里，我们设计了一系列芘-4，5，9，10-四酮COF（PT-COF）和碳纳米管（CNT）复合材料（表示为PT-COFX，其中X = CNT的10，30和50重量%）来解决这些挑战。在这些复合材料中，PT-COF 50在200 mA g-1的电流密度下实现了标准化为活性COF材料的高达280 mAh g-1的容量，这是迄今为止报道的基于COF的复合阴极电极的最高容量。此外，PT-COF 50表现出优异的倍率性能，在5000 mA g-1（18.5C）下提供229 mAh g-1的容量。使用操作拉曼显微镜的氧化还原活性羰基的PT-COF的可逆转化进行了测定，这合理化的总体4 e-/4 Li+氧化还原过程每个芘-4，5，9，10-四酮单元，占其作为锂离子电池电极的上级性能。
Electrochemically active covalent organic frameworks (COFs) are promising electrode materials for Li-ion batteries. However, improving the specific capacities of COF-based electrodes requires materials with increased conductivity and a higher concentration of redox-active groups. Here, we designed a series of pyrene-4,5,9,10-tetraone COF (PT-COF) and carbon nanotube (CNT) composites (denoted as PT-COFX, where X = 10, 30, and 50 wt % of CNT) to address these challenges. Among the composites, PT-COF50 achieved a capacity of up to 280 mAh g–1 as normalized to the active COF material at a current density of 200 mA g–1, which is the highest capacity reported for a COF-based composite cathode electrode to date. Furthermore, PT-COF50 exhibited excellent rate performance, delivering a capacity of 229 mAh g–1 at 5000 mA g–1 (18.5C). Using operando Raman microscopy the reversible transformation of the redox-active carbonyl groups of PT-COF was determined, which rationalizes an overall 4 e–/4 Li+ redox process per pyrene-4,5,9,10-tetraone unit, accounting for its superior performance as a Li-ion battery electrode.
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