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铁沉积诱导缺氧钛酸盐纳米管增强过一硫酸盐活化及对扑热息痛的降解:机理、水化学效应及理论计算。

Oxygen defective titanate nanotubes induced by iron deposition for enhanced peroxymonosulfate activation and acetaminophen degradation: Mechanisms, water chemistry effects, and theoretical calculation.

机构信息

School of Environmental Science and engineering, Taiyuan University of Science and Technology, Taiyuan, Shanxi 030024, China.

The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China; State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems, Peking University, Beijing 100871, China.

出版信息

J Hazard Mater. 2021 Sep 15;418:126180. doi: 10.1016/j.jhazmat.2021.126180. Epub 2021 May 27.

Abstract

The large consumption of acetaminophen (APAP) worldwide and unsatisfactory treatment efficiencies by conventional wastewater treatment processes give rise to the seeking of new technology for its effective removal. Herein, we proposed a facile one-step hydrothermal method to synthesize defective iron deposited titanate nanotubes (Fe/TNTs) for peroxymonosulfate (PMS) activation and APAP degradation. The retarded first-order reaction rate of APAP degradation by Fe/TNTs was 5.1 times higher than that of neat TNTs. Characterizations indicated iron deposition effectively induced oxygen vacancies and Ti, facilitating the electrical conductivity and PMS binding affinity of Fe/TNTs. Besides, oxygen vacancies could act as an electron mediator through PMS activation by iron. Moreover, the formation of Fe-O-Ti bond facilitated the synergistic redox coupling between Fe and Ti, further enhancing the PMS activation. SO was the major radical, causing C-N bond cleavage and decreasing the overall toxicity. In contrast, APAP degradation by neat TNTs-PMS system mainly works through nonradical reaction. The Fe/TNTs activated PMS showed desired APAP removal under mild water chemistry conditions and good reusability. This work is expected to expand the potential application of titanate nanomaterials for PMS activation, and shed light on facile synthesis of oxygen defective materials for sulfate-radical-based advanced oxidation processes.

摘要

全球范围内对乙酰氨基酚(APAP)的大量消耗,以及传统废水处理工艺不尽如人意的处理效率,促使人们寻求新的技术来有效去除它。在此,我们提出了一种简便的一步水热法来合成缺陷型铁沉积钛酸盐纳米管(Fe/TNTs),用于过一硫酸盐(PMS)的活化和 APAP 的降解。Fe/TNTs 对 APAP 降解的一级反应速率常数比纯 TNTs 慢 5.1 倍。表征表明,铁沉积有效地诱导了氧空位和 Ti,提高了 Fe/TNTs 的电导率和 PMS 结合亲和力。此外,氧空位可以通过铁活化 PMS 充当电子介体。此外,Fe-O-Ti 键的形成促进了 Fe 和 Ti 之间的协同氧化还原偶联,进一步增强了 PMS 的活化。SO 是主要的自由基,导致 C-N 键断裂,降低了整体毒性。相比之下,纯 TNTs-PMS 体系中 APAP 的降解主要通过非自由基反应进行。在温和的水化学条件下,Fe/TNTs 活化的 PMS 表现出良好的 APAP 去除效果,且具有良好的可重复使用性。这项工作有望扩展钛酸盐纳米材料在 PMS 活化方面的潜在应用,并为基于硫酸盐自由基的高级氧化工艺中氧缺陷材料的简便合成提供启示。

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