富缺陷N/O共掺杂多孔炭框架材料作为高性能钾、钠离子电池负极材料

Defect-rich N/O-co-doped porous carbon frameworks as anodes for superior potassium and sodium-ion batteries

  • 摘要: 炭材料因其高导电性、高化学稳定性和有效缓解体积变化的能力成为钠、钾离子电池最富前景的负极材料。本文报道了一种由N/O共掺杂介孔碳纳米片组成的富缺陷N/O共掺杂多孔炭框架材料 (简称DRPCF)。其中DRPCF-2/1-700拥有最高的比表面积、孔体积和最高的N/O含量的活性缺陷位点。因此DRPCF-2/1-700 展现出超高的赝电容行为主导的钠、钾离子存储行为。作为钠、钾离子电池的负极材料,DRPCF-2/1-700均展现出高倍率和长循环性能,在1 A g−1电流密度下分别900和1200圈后质量比容量仍保持在328.2和321.5 mAh g−1,以上性能优于大部分已报道的碳基负极材料。非原位拉曼光谱分析结果进一步证实了钾、钠离子从电化学活性缺陷位点的填充和脱除是赋予DRPCF-2/1-700高容量、超高倍率和超长循环性能的主要原因。

     

    Abstract: Carbon with its high electrical conductivity, excellent chemical stability, and structure ability is the most promising anode material for sodium and potassium ion batteries. We developed a defect-rich porous carbon framework (DRPCF) built with N/O-co-doped mesoporous nanosheets and containing many defects using porous g-C3N4 (PCN) and dopamine (DA) as raw materials. We prepared samples with PCN/DA mass ratios of 1/1, 2/1 and 3/1 and found that the one with a mass ratio of 2/1 and a carbonization temperature of 700 °C in an Ar atmosphere (DRPCF-2/1-700), had a large specific surface area with an enormous pore volume and a large number of N/O heteroatom active defect sites. Because of this, it had the best pseudocapacitive sodium and potassium ion storage performance. A half battery of Na//DRPCF-2/1-700 maintained a capacity of 328.2 mAh g−1 after being cycled at 1 A g−1 for 900 cycles, and a half battery of K//DRPC-2/1-700 maintained a capacity of 321.5 mAh g−1 after being cycled at 1 A g−1 for 1200 cycles. The rate capability and cycling stability achieved by DRPCF-2/1-700 outperforms most reported carbon materials. Finally, ex-situ Raman spectroscopy analysis result confirms that the filling and removing of K+ and Na+ from the electrochemically active defects are responsible for the high capacity, superior rate and cycling performance of the DRPCF-2/1-700 sample.

     

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