期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 144, 期 21, 页码 9434-9442出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c02196
关键词
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资金
- EPSRC [EP/R020744/1, EP/V026887/1, EP/N004884/1]
- Leverhulme Trust via the Leverhulme Research Centre for Functional Materials Design
- China Scholarship Council (CSC)
- University of Liverpool Graduate Association (Hong Kong)
This study designed a series of pyrene-4,5,9,10-tetraone COF and carbon nanotube composites to improve the specific capacity of COF-based electrodes. Among the composites, PT-COF50 achieved the highest capacity and demonstrated excellent rate performance. The reversible transformation of the redox-active carbonyl groups of PT-COF was determined using operando Raman microscopy.
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, PTCOF-50 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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