催化学报

催化学报 ›› 2014, Vol. 35 ›› Issue (6): 896-905.DOI: 10.1016/S1872-2067(14)60103-0

• 研究论文 • 上一篇    下一篇

Catalytic performance of heteroatom-modified carbon nanotubes in advanced oxidation processes

João Restivo, Raquel P. Rocha, Adrián M. T. Silva, José J. M. Órfão, Manuel F. R. Pereira, José L. Figueiredo   

  1. Laboratory of Catalysis and Materials-Associate Laboratory LSRE/LCM, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias, 4200-465 Porto, Portugal
  • 收稿日期:2014-04-03 修回日期:2014-04-17 出版日期:2014-05-30 发布日期:2014-06-03
  • 通讯作者: José L. Figueiredo
  • 基金资助:

    This work was supported by FREECATS, the European Union 7th FP (2007-2013) grant no. 280658, PEst-C/EQB/LA0020/2013, FEDER through COMPETE-Programa Operacional Factores de Competitividade, by FCT-Fundação para a Ciência e a Tecnologia, NORTE-07-0124-FEDER-0000015, NORTE-07-0162-FEDER-000050, QREN, ON2, FEDER.

Catalytic performance of heteroatom-modified carbon nanotubes in advanced oxidation processes

João Restivo, Raquel P. Rocha, Adrián M. T. Silva, José J. M. Órfão, Manuel F. R. Pereira, José L. Figueiredo   

  1. Laboratory of Catalysis and Materials-Associate Laboratory LSRE/LCM, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias, 4200-465 Porto, Portugal
  • Received:2014-04-03 Revised:2014-04-17 Online:2014-05-30 Published:2014-06-03
  • Supported by:

    This work was supported by FREECATS, the European Union 7th FP (2007-2013) grant no. 280658, PEst-C/EQB/LA0020/2013, FEDER through COMPETE-Programa Operacional Factores de Competitividade, by FCT-Fundação para a Ciência e a Tecnologia, NORTE-07-0124-FEDER-0000015, NORTE-07-0162-FEDER-000050, QREN, ON2, FEDER.

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摘要：

Multi-walled carbon nanotubes (CNTs) were submitted to chemical and thermal treatments in order to incorporate different heteroatoms on the surface. O-, S-and N-containing groups were successfully introduced onto the CNTs without significant changes of the textural properties. The catalytic activity of these heteroatom-modified CNTs was studied in two liquid phase oxidation processes: catalytic ozonation and catalytic wet air oxidation (CWAO), using oxalic acid and phenol as model compounds. In both cases, the presence of strongly acidic O-containing groups was found to decrease the catalytic activity of the CNTs. On the other hand, the introduction of S species (mainly sulfonic acids) enhanced the removal rate of the model compounds, particularly in the CWAO of phenol. Additional experiments were performed with a radical scavenger and sodium persulfate, in order to clarify the reaction mechanism. Nitrogen functionalities improve the catalytic performance of the original CNTs, regardless of the process or of the pollutant.

关键词: Advanced oxidation processes, Catalytic ozonation, Catalytic wet air oxidation, Sulfur groups, Nitrogen groups, Oxygen groups, Carbon nanotubes, Surface chemistry

Abstract:

Multi-walled carbon nanotubes (CNTs) were submitted to chemical and thermal treatments in order to incorporate different heteroatoms on the surface. O-, S-and N-containing groups were successfully introduced onto the CNTs without significant changes of the textural properties. The catalytic activity of these heteroatom-modified CNTs was studied in two liquid phase oxidation processes: catalytic ozonation and catalytic wet air oxidation (CWAO), using oxalic acid and phenol as model compounds. In both cases, the presence of strongly acidic O-containing groups was found to decrease the catalytic activity of the CNTs. On the other hand, the introduction of S species (mainly sulfonic acids) enhanced the removal rate of the model compounds, particularly in the CWAO of phenol. Additional experiments were performed with a radical scavenger and sodium persulfate, in order to clarify the reaction mechanism. Nitrogen functionalities improve the catalytic performance of the original CNTs, regardless of the process or of the pollutant.

Key words: Advanced oxidation processes, Catalytic ozonation, Catalytic wet air oxidation, Sulfur groups, Nitrogen groups, Oxygen groups, Carbon nanotubes, Surface chemistry