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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:催化过氧单硫酸盐活化过程中碳纳米管和氮掺杂碳纳米管的失活和再生,用于苯酚降解:表面功能的变化

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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 NaBH _(4) 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:研究了碳纳米管(CNT)和N掺杂碳纳米管(NCNT)在催化过氧单硫酸盐(PMS)活化过程中苯酚降解的再利用,失活和再生。结果表明,对于催化PMS活化,在CNT和NCNT上均观察到明显的失活,从而导致催化剂表面功能的明显变化。催化PMS活化导致CNT和NCNT的含氧官能团显着增加,零电荷点(PZCs)降低。 CNT的催化活性在很大程度上取决于初始PMS浓度,但与初始苯酚浓度无关。此外,CNT活性对PMS初始浓度的依赖性非常符合Langmuir-Hinshelwood模型,表明吸附的PMS的催化活化是速率控制步骤。对于用过的CNT和NCNT,通过NaBH_(4)进行化学还原或在惰性气氛下进行热处理再生可有效去除表面含O的官能团并增强PZC,恢复其催化活性。同时,随着再生处理,NCNT的含氮官能团降低,对催化剂的再生产生负面影响。目前的发现表明,表面功能与催化剂的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。

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