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钴掺杂的氧氯化铁作为高效的非均相 Fenton 催化剂用于降解扑热息痛和非那西汀。

Cobalt doped iron oxychloride as efficient heterogeneous Fenton catalyst for degradation of paracetamol and phenacetin.

机构信息

School of Civil Engineering, Southeast University, Nanjing, 210096, China; Key Laboratory of Concrete and Prestressed Concrete Structures of the Ministry of Education, Southeast University, Nanjing, 210096, China.

School of Civil Engineering, Southeast University, Nanjing, 210096, China.

出版信息

Chemosphere. 2021 Jan;263:127989. doi: 10.1016/j.chemosphere.2020.127989. Epub 2020 Aug 29.

DOI:10.1016/j.chemosphere.2020.127989
PMID:33297032
Abstract

Cobalt doped iron oxychloride (Co-FeOCl) was synthesized and employed as catalyst in Fenton degradation of paracetamol (APAP) and phenacetin (PNCT) for the first time. The catalytic performance was evaluated by means of various parameters including catalyst load, hydrogen peroxide (HO) dose and pH value. The high removal of APAP (87.5%) and PNCT (76.0%) was obtained under conditions of 0.2 g/L Co-FeOCl and 0.5 mM HO at pH 7.0, with calculated pseudo-first order kinetic constants of 0.031 min for APAP and 0.023 min for PNCT. Particularly, quenching tests and in situ electron spin resonance (ESR) tests were employed for the identification of the reactive oxygen species (ROS) in system. Hydroxyl radical (·OH) and superoxide radical (O·) were the primary ROS in Co-FeOCl/HO system. A possible mechanism for HO activation by Co-FeOCl catalyst was proposed as well. Finally, the formation of typical disinfection by-products (DBPs) decreased slightly in Co-FeOCl/HO pre-oxidation. However, stability and reusability of Co-FeOCl were deactivated in the consecutive three cycles.

摘要

首次合成了钴掺杂的氧氯化铁(Co-FeOCl),并将其用作芬顿降解对乙酰氨基酚(APAP)和非那西汀(PNCT)的催化剂。通过各种参数(包括催化剂负载量、过氧化氢(HO)剂量和 pH 值)评估了催化性能。在 0.2 g/L Co-FeOCl 和 0.5 mM HO 的条件下,在 pH 7.0 下,APAP(87.5%)和 PNCT(76.0%)的去除率很高,计算出的 APAP 的拟一级动力学常数为 0.031 min,PNCT 的为 0.023 min。特别地,采用猝灭试验和原位电子自旋共振(ESR)试验来鉴定体系中的活性氧物种(ROS)。羟基自由基(·OH)和超氧自由基(O·)是 Co-FeOCl/HO 体系中的主要 ROS。还提出了 Co-FeOCl 催化剂活化 HO 的可能机制。最后,Co-FeOCl/HO 预氧化过程中典型消毒副产物(DBP)的形成略有减少。然而,在连续三个循环中,Co-FeOCl 的稳定性和可重复使用性被失活。

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