Journal of Hazardous Materials ( IF 13.6 ) Pub Date : 2021-10-22 , DOI: 10.1016/j.jhazmat.2021.127569 Dongdong He 1 , Ke Zhu 1 , Jin Huang 1 , Yaqian Shen 1 , Lele Lei 1 , Hongmei He 1 , Wenjin Chen 1
Heteroatoms doped carbon materials are widely used in the advanced oxidation process (AOPs) to remove organic pollutants in water due to the synergies effect between different heteroatoms. In this study, a novel kind of N, S co-doped magnetic mesoporous carbon nanosheets (Fe@NS-C) was prepared by simple one-step pyrolysis. Further, the influence of doping amount of S (L-methionine) and N (melamine) on catalytic activity was studied, the optimized sample Fe@NS-C-2-12/PMS showed a satisfying degradation ( 91.07%) for high concentrations of tetracycline (80 mg/L TC) in 10 min, which was attributed to the proper ratio of S content to N content (S(at.%)/ N(at.%) = 0.2097) in the sample could better play its synergistic effect by XPS analysis. The Fe@NS-C-2-12/ PMS system also exhibited satisfactory degradation effects in a wide pH range (3−10) and the existence of inorganic ions and humic acid. Then, the degradation mechanisms were mainly through the non-radical pathway (1O2 and electron transfer) and the major active sites were pyridinic N compared to thiophene S, CO, and Fe-Nx. This study could inspire the design of high-performance active and low-cost heteroatomic doping nano-magnetic catalysts for PMS-based waste treatment.
中文翻译:
N、S共掺杂磁性介孔碳纳米片活化过一硫酸盐快速降解四环素:协同效应及机理
由于不同杂原子之间的协同作用,杂原子掺杂碳材料广泛用于高级氧化工艺(AOPs)去除水中的有机污染物。在这项研究中,通过简单的一步热解制备了一种新型的 N、S 共掺杂磁性介孔碳纳米片(Fe@NS-C)。此外,研究了S( L-蛋氨酸)和N(三聚氰胺)的掺杂量对催化活性的影响,优化后的样品Fe@NS-C-2-12/PMS在高浓度下表现出令人满意的降解(91.07%)四环素 (80 mg/L TC) 在 10 分钟内,这归因于 S 含量与 N 含量的适当比率 (S(at.%)/N(at.%) = 0.2097)通过XPS分析可以更好地发挥其协同作用。Fe@NS-C-2-12/PMS体系在较宽的pH范围(3-10)和无机离子和腐植酸的存在下也表现出令人满意的降解效果。然后,降解机制主要通过非自由基途径(1 O 2和电子转移),与噻吩S、CO和Fe-N x相比,主要活性位点是吡啶N。这项研究可以启发设计用于基于 PMS 的废物处理的高性能活性和低成本杂原子掺杂纳米磁性催化剂。