能源化学(英文版)

能源化学(英文版) ›› 2020, Vol. 49 ›› Issue (10): 179-188.DOI: 10.1016/j.jechem.2020.02.024

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SiO2 stabilizes electrochemically active nitrogen in few-layer carbon electrodes of extraordinary capacitance

Feng Xua,b, Tianquan Lina, Jian Huanga, I-Wei Chenc, Fuqiang Huanga,d   

  1. a State Key Laboratory of High Performance Ceramics and Superfine Microstructure,Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai 200050,China;
    b University of Chinese Academy of Sciences,19 Yuquan Road,Beijing 100049,China;
    c Department of Materials Science and Engineering,University of Pennsylvania,Philadelphia,PA 19104,USA;
    d College of Chemistry and Molecular Engineering,Peking University,Beijing 100871,China
  • 收稿日期:2020-01-09 修回日期:2020-02-18 出版日期:2020-10-15 发布日期:2020-12-18
  • 通讯作者: Fuqiang Huang
  • 基金资助:
    Research of F.Xu,T.Lin,J.Huang and F.Huang was supported by the National Key Research and Development Program of China(Grant no.2016YFB0901600),the National Natural Science Foundation of China(Grant nos.51922103 and 51672301),and the Key Research Program of Chinese Academy of Sciences(Grant no.QYZDJSSW-JSC013).

SiO2 stabilizes electrochemically active nitrogen in few-layer carbon electrodes of extraordinary capacitance

Feng Xua,b, Tianquan Lina, Jian Huanga, I-Wei Chenc, Fuqiang Huanga,d   

  1. a State Key Laboratory of High Performance Ceramics and Superfine Microstructure,Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai 200050,China;
    b University of Chinese Academy of Sciences,19 Yuquan Road,Beijing 100049,China;
    c Department of Materials Science and Engineering,University of Pennsylvania,Philadelphia,PA 19104,USA;
    d College of Chemistry and Molecular Engineering,Peking University,Beijing 100871,China
  • Received:2020-01-09 Revised:2020-02-18 Online:2020-10-15 Published:2020-12-18
  • Contact: Fuqiang Huang
  • Supported by:
    Research of F.Xu,T.Lin,J.Huang and F.Huang was supported by the National Key Research and Development Program of China(Grant no.2016YFB0901600),the National Natural Science Foundation of China(Grant nos.51922103 and 51672301),and the Key Research Program of Chinese Academy of Sciences(Grant no.QYZDJSSW-JSC013).

摘要： Pyrrolic and pyridinic N dopants can dramatically increase the electrochemical activities of carbon and conducting polymers.Although N-doped conducting polymers suffer from rapid degradation,their carbon counterpart of extraordinary capacitance has remarkable rate performance and cycling endurance thanks to carbon's excellent electrical conductivity.But high nitrogen content and high electrical conductivity are difficult to achieve in a high-surface-area carbon,because the high chemical vapor deposition (CVD) temperature required for obtaining high conductivity also destabilizes under-coordinated pyrrolic and pyridinic nitrogen and tends to lower the surface area.Here we resolve this dilemma by using SiO2 as an effective N-fixation additive,which stabilizes the N-rich nano few-layer sp2-carbon construct in 1000℃ CVD.This enables a scalable sol-gel/CVD fabrication process for few-layer carbon electrodes of extraordinary capacitance (690 F g-1).The electrodes have excellent rate performance and can maintain 90% of their initial capacitance after 30,000 cycles,thus potentially suitable for practical applications.

关键词: Electrochemical capacitors, Carbon electrodes, Extraordinary capacitance, SiO2 stabilized nitrogen

Abstract: Pyrrolic and pyridinic N dopants can dramatically increase the electrochemical activities of carbon and conducting polymers.Although N-doped conducting polymers suffer from rapid degradation,their carbon counterpart of extraordinary capacitance has remarkable rate performance and cycling endurance thanks to carbon's excellent electrical conductivity.But high nitrogen content and high electrical conductivity are difficult to achieve in a high-surface-area carbon,because the high chemical vapor deposition (CVD) temperature required for obtaining high conductivity also destabilizes under-coordinated pyrrolic and pyridinic nitrogen and tends to lower the surface area.Here we resolve this dilemma by using SiO2 as an effective N-fixation additive,which stabilizes the N-rich nano few-layer sp2-carbon construct in 1000℃ CVD.This enables a scalable sol-gel/CVD fabrication process for few-layer carbon electrodes of extraordinary capacitance (690 F g-1).The electrodes have excellent rate performance and can maintain 90% of their initial capacitance after 30,000 cycles,thus potentially suitable for practical applications.

Key words: Electrochemical capacitors, Carbon electrodes, Extraordinary capacitance, SiO2 stabilized nitrogen