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Deactivation and regeneration of carbon nanotubes and nitrogen-doped carbon nanotubes in catalytic peroxymonosulfate activation for phenol degradation: variation of surface functionalities

机译:碳纳米管和氮掺杂碳纳米管在催化过氧键硫酸盐活化中的碳纳米管和氮掺杂碳纳米管的去激活和再生苯酚降解:表面函数变异

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摘要

The reuse, deactivation and regeneration of carbon nanotubes (CNT) and N-doped carbon nanotubes (NCNT) were studied in catalytic peroxymonosulfate (PMS) activation for phenol degradation. The results showed that for catalytic PMS activation, marked deactivation was observed on both CNT and NCNT, resulting in marked variation of the surface functionalities of the catalysts. Catalytic PMS activation led to markedly increased oxygen-containing functionalities and decreased points of zero charge (PZCs) of CNT and NCNT. The catalytic activity of CNT was strongly dependent on the initial PMS concentration but was independent of the initial phenol concentration. Furthermore, the dependency of the CNT activity on the initial PMS concentration closely followed the Langmuir-Hinshelwood model, indicating that the catalytic activation of adsorbed PMS was the rate controlling step. For the used CNT and NCNT, chemical reduction by NaBH4 or thermal treatment regeneration under inert atmosphere could effectively remove surface O-containing functionalities and enhance PZCs, restoring their catalytic activities; meanwhile, the N-containing functionalities of NCNT decreased with regeneration treatment, resulting in a negative impact on catalyst regeneration. The present findings indicate that surface functionalities are closely correlated with catalyst deactivation and regeneration, playing crucial roles in the catalytic activation of PMS.
机译:碳纳米管(CNT)和N-掺杂碳纳米管(NCNT)的再利用,停用和再生在催化过氧键硫酸盐(PMS)活化中研究了苯酚降解。结果表明,对于催化PMS活化,在CNT和NCNT上观察到标记的去激活,导致催化剂的表面官能团的显着变化。催化PMS活化导致含氧功能和CNT和NCNT的含氧函数和下降点(PZC)的下降点。 CNT的催化活性强烈依赖于初始PMS浓度,但与初始酚浓度无关。此外,CNT活性对初始PMS浓度的依赖性紧密遵循Langmuir-Hinshelwood模型,表明吸附的PMS的催化活化是速率控制步骤。对于使用的CNT和NCNT,惰性气氛下的NaBH 4或热处理再生的化学降低可以有效去除含表面O的功能,并增强PZC,恢复其催化活性;同时,NCNT的含N官能团随着再生处理而降低,导致对催化剂再生产生负面影响。本研究结果表明,表面功能与催化剂失活和再生密切相关,在PMS的催化活化中起着至关重要的作用。

著录项

  • 来源
    《RSC Advances》 |2019年第2期|共10页
  • 作者单位

    Nanjing Univ Sch Environm Jiangsu Key Lab Vehicle Emiss Control State Key Lab Pollut Control &

    Resource Reuse Nanjing 210093 Jiangsu Peoples R China;

    Nanjing Univ Sch Environm Jiangsu Key Lab Vehicle Emiss Control State Key Lab Pollut Control &

    Resource Reuse Nanjing 210093 Jiangsu Peoples R China;

    Nanjing Univ Sch Environm Jiangsu Key Lab Vehicle Emiss Control State Key Lab Pollut Control &

    Resource Reuse Nanjing 210093 Jiangsu Peoples R China;

    Nanjing Univ Sch Environm Jiangsu Key Lab Vehicle Emiss Control State Key Lab Pollut Control &

    Resource Reuse Nanjing 210093 Jiangsu Peoples R China;

    Nanjing Univ Sch Environm Jiangsu Key Lab Vehicle Emiss Control State Key Lab Pollut Control &

    Resource Reuse Nanjing 210093 Jiangsu Peoples R China;

    Nanjing Univ Sch Environm Jiangsu Key Lab Vehicle Emiss Control State Key Lab Pollut Control &

    Resource Reuse Nanjing 210093 Jiangsu Peoples R China;

    Nanjing Univ Sch Environm Jiangsu Key Lab Vehicle Emiss Control State Key Lab Pollut Control &

    Resource Reuse Nanjing 210093 Jiangsu Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
  • 关键词

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