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Fe3O4 磁性纳米粒子作为过一硫酸盐的非均相活化剂诱导对乙酰氨基酚的自由基降解。

Radical induced degradation of acetaminophen with Fe3O4 magnetic nanoparticles as heterogeneous activator of peroxymonosulfate.

机构信息

State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai City 200092, China.

State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai City 200092, China.

出版信息

J Hazard Mater. 2014 Jul 15;276:452-60. doi: 10.1016/j.jhazmat.2014.05.068. Epub 2014 Jun 2.

DOI:10.1016/j.jhazmat.2014.05.068
PMID:24929305
Abstract

Magnetic nano-scaled particles Fe3O4 were studied for the activation of peroxymonosulfate (PMS) to generate active radicals for degradation of acetaminophen (APAP) in water. The Fe3O4 MNPs were found to effectively catalyze PMS for removal of APAP, and the reactions well followed a pseudo-first-order kinetics pattern (R(2)>0.95). Within 120min, approximately 75% of 10ppm APAP was accomplished by 0.2mM PMS in the presence of 0.8g/L Fe3O4 MNPs with little Fe(3+) leaching (<4μg/L). Higher Fe3O4 MNP dose, lower initial APAP concentration, neutral pH, and higher reaction temperature favored the APAP degradation. The production of sulfate radicals and hydroxyl radicals was validated through two ways: (1) indirectly from the scavenging tests with scavenging agents, tert-butyl alcohol (TBA) and ethanol (EtOH); (2) directly from the electron paramagnetic resonance (ESR) tests with 0.1M 5,5-dimethyl-1-pyrrolidine N-oxide (DMPO). Plausible mechanisms on the radical generation from Fe3O4 MNP activation of PMS are proposed based on the results of radical identification tests and XPS analysis. It appeared that Fe(2+)Fe(3+) on the catalyst surface was responsible for the radical generation. The results demonstrated that Fe3O4 MNPs activated PMS is a promising technology for water pollution caused by contaminants such as pharmaceuticals.

摘要

磁性纳米级 Fe3O4 颗粒被研究用于激活过一硫酸盐 (PMS) 以生成活性自由基,用于降解水中的扑热息痛 (APAP)。研究发现,Fe3O4 MNPs 能有效地催化 PMS 去除 APAP,反应很好地遵循了拟一级动力学模式(R(2)>0.95)。在 120min 内,在 0.8g/L Fe3O4 MNPs 存在下,用 0.2mM PMS 处理 10ppm 的 APAP 时,约有 75%的 APAP 被去除,Fe(3+)浸出量很少(<4μg/L)。更高的 Fe3O4 MNP 剂量、更低的初始 APAP 浓度、中性 pH 值和更高的反应温度有利于 APAP 的降解。通过两种方式验证了硫酸根自由基和羟基自由基的生成:(1)通过与猝灭剂叔丁醇 (TBA) 和乙醇 (EtOH) 的猝灭试验间接验证;(2)通过电子顺磁共振 (ESR) 试验直接用 0.1M 5,5-二甲基-1-吡咯烷 N-氧化物 (DMPO) 验证。根据自由基识别试验和 XPS 分析的结果,提出了基于 Fe3O4 MNP 活化 PMS 生成自由基的可能机制。似乎是催化剂表面上的 Fe(2+)Fe(3+) 负责生成自由基。结果表明,Fe3O4 MNPs 激活 PMS 是一种很有前途的技术,可用于处理由药物等污染物引起的水污染问题。

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