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Nitrogen and sulfur co-doped mesoporous carbon as an efficient peracetic acid activator for the degradation of 4-chlorophenol: A nonradical mechanism dominated by singlet oxygen
Separation and Purification Technology ( IF 8.6 ) Pub Date : 2024-05-08 , DOI: 10.1016/j.seppur.2024.127843
Guizhou Xu , Zunyao Wang , Lin Sun , Aimin Li , Xianchuan Xie , Xueyuan Gu

Metal-free peracetic acid (PAA) activators are urgently required due to their low toxicity. Heteroatom doping is beneficial to improve the catalytic performance of carbon materials, but the activation performance of doped carbon materials on PAA and the underlying mechanism have not been reported. Herein, nitrogen and sulfur co-doped mesoporous carbons (NS-MC-x, with x representing the mass ratio of thiourea:mesoporous carbon) were fabricated and used as efficient PAA activators for 4-chlorophenol (4-CP) degradation. The NS-MC-1.0/PAA system can remove > 95 % of 4-CP within 10 min, far more than the MC/PAA system. Co-existing anions show no effect on the degradation of 4-CP, whereas humic acid has a certain degree of inhibition. Singlet oxygen (O) primarily drives the degradation of 4-CP, with a secondary contribution from a direct electron transfer process mediated by reactive surface complexes, while the contribution of radicals is minimal. In addition, NS-MC-1.0 exhibits excellent reusability for PAA activation, which is conductive to its practical application. This study facilitates further research on metal-free catalysts for PAA activation and offers fresh perspectives on the utilization of PAA in degrading emerging pollutants.

中文翻译:


氮和硫共掺杂介孔碳作为有效的过乙酸活化剂降解4-氯苯酚:以单线态氧为主的非自由基机制



由于其低毒性,迫切需要无金属的过乙酸(PAA)活化剂。杂原子掺杂有利于提高碳材料的催化性能,但掺杂碳材料对PAA的活化性能及其机制尚未见报道。在此,制备了氮和硫共掺杂介孔碳(NS-MC-x,其中x代表硫脲:介孔碳的质量比)并用作4-氯酚(4-CP)降解的有效PAA活化剂。 NS-MC-1.0/PAA系统可以在10分钟内去除>95%的4-CP,远远超过MC/PAA系统。共存阴离子对4-CP的降解没有影响,而腐植酸则有一定程度的抑制作用。单线态氧 (O) 主要驱动 4-CP 的降解,其次是由反应性表面复合物介导的直接电子转移过程,而自由基的贡献很小。此外,NS-MC-1.0对PAA活化具有良好的可重复使用性,有利于其实际应用。这项研究促进了对用于 PAA 活化的无金属催化剂的进一步研究,并为利用 PAA 降解新兴污染物提供了新的视角。
更新日期:2024-05-08
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