催化学报 ›› 2014, Vol. 35 ›› Issue (6): 884-890.DOI: 10.1016/S1872-2067(14)60108-X

• 研究论文 • 上一篇    下一篇

Solution phase synthesis of halogenated graphene and the electrocatalytic activity for oxygen reduction reaction

Kuang-Hsu Wua, Da-Wei Wanga,b, Qingcong Zenga, Yang Lia, Ian R. Gentlea   

  1. a School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane 4072, Australia;
    b School of Chemical Engineering, UNSW Australia (The University of New South Wales), Sydney, NSW 2052, Australia
  • 收稿日期:2014-04-03 修回日期:2014-04-18 出版日期:2014-05-30 发布日期:2014-06-03
  • 通讯作者: Da-Wei Wang,Ian R. Gentle

Solution phase synthesis of halogenated graphene and the electrocatalytic activity for oxygen reduction reaction

Kuang-Hsu Wua, Da-Wei Wanga,b, Qingcong Zenga, Yang Lia, Ian R. Gentlea   

  1. a School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane 4072, Australia;
    b School of Chemical Engineering, UNSW Australia (The University of New South Wales), Sydney, NSW 2052, Australia
  • Received:2014-04-03 Revised:2014-04-18 Online:2014-05-30 Published:2014-06-03

摘要:

Metal-free carbon electrocatalyts for the oxygen reduction reaction (ORR) are attractive for their high activity and economic advantages. However, the origin of the activity has never been clearly elucidated in a systematic manner. Halogen group elements are good candidates for elucidating the effect, although it has been a difficult task due to safety issues. In this report, we demonstrate the synthesis of Cl-, Br-and I-doped reduced graphene oxide through two solution phase syntheses. We have evaluated the effectiveness of doping and performed electrochemical measurements of the ORR activity on these halogenated graphene materials. Our results suggest that the high electronegativity of the dopant is not the key factor for high ORR activity; both Br-and I-doped graphene promoted ORR more efficiently than Cl-doped graphene. Furthermore, an unexpected sulfur-doping in acidic conditions suggests that a high level of sulfide can degrade the ORR activity of the graphene material.

关键词: Halogen-doping, Sulfur-doping, Graphene, Oxygen reduction reaction, Electrocatalyst

Abstract:

Metal-free carbon electrocatalyts for the oxygen reduction reaction (ORR) are attractive for their high activity and economic advantages. However, the origin of the activity has never been clearly elucidated in a systematic manner. Halogen group elements are good candidates for elucidating the effect, although it has been a difficult task due to safety issues. In this report, we demonstrate the synthesis of Cl-, Br-and I-doped reduced graphene oxide through two solution phase syntheses. We have evaluated the effectiveness of doping and performed electrochemical measurements of the ORR activity on these halogenated graphene materials. Our results suggest that the high electronegativity of the dopant is not the key factor for high ORR activity; both Br-and I-doped graphene promoted ORR more efficiently than Cl-doped graphene. Furthermore, an unexpected sulfur-doping in acidic conditions suggests that a high level of sulfide can degrade the ORR activity of the graphene material.

Key words: Halogen-doping, Sulfur-doping, Graphene, Oxygen reduction reaction, Electrocatalyst