• Little, Marc
• Cooper, Andrew I.
• Gao, Hui
• Browning, Nigel D.
• Hardwick, Laurence J.
• Neale, Alex R.
• Yang, Haofan
• Wang, Xue
• Clowes, Rob
• Zhu, Qiang
• Bahri, Mounib
• Xu, Yongjie

Abstract

<p>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, whereX = 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). Usingoperando 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. </p>

Topics

• density
• impedance spectroscopy
• Carbon
• nanotube
• composite
• current density
• Raman microscopy