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羟胺介导的基于废磷酸铁锂动力电池衍生的海胆状催化剂的类芬顿界面反应动力学

Hydroxylamine mediated Fenton-like interfacial reaction dynamics on sea urchin-like catalyst derived from spent LiFePO battery.

作者信息

Zou Wensong, Li Jing, Wang Ranhao, Ma Jingyi, Chen Zhijie, Duan Lele, Mi Hongwei, Chen Hong

机构信息

State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control, Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials, Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, PR China; School of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, PR China.

State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control, Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials, Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, PR China.

出版信息

J Hazard Mater. 2022 Jun 5;431:128590. doi: 10.1016/j.jhazmat.2022.128590. Epub 2022 Feb 26.

DOI:10.1016/j.jhazmat.2022.128590
PMID:35247735
Abstract

Herein, we converted spent LiFePO battery to the sea urchin-like material (SULM) with a highly efficient and environment-friendly method, which can contribute to building a zero-waste city. With SULM as a Fenton-like catalyst, a highly-efficient degradation process was realized for organic pollutants with interface and solution synergistic effect. In our SULM+NHOH+HO Fenton-like system, NHOH can effectively promote the interface iron (Fe(Ⅲ)/Fe(Ⅱ)) and solution iron (Fe(Ⅲ)/Fe(Ⅱ)) redox cycle, thus promoting the generation of reactive oxygen species (ROS). However, the ROS generation process and organic pollutants degradation pathway with the presence of NHOH remains a puzzle. Here the detailed ROS generation mechanism and pollutants degradation pathway have been illustrated carefully based on experimental exploration and characterization. Therein, hydroxyl radicals (·OH) and singlet oxygen (O) are the main ROS for oxidizing and degrading organic pollutants. Notably, O can be converted from superoxide radicals (·O) in SULM+NHOH+HO system. This study not only demonstrates the strategy of "trash-to-treasure" and "waste-to-control-waste" to simultaneously reduce the hazardous release from industrial solid waste and organic wastewater, it also provides new mechanistic insights for NHOH mediated Fenton-like redox system.

摘要

在此,我们采用一种高效且环保的方法将废旧磷酸铁锂电池转化为海胆状材料(SULM),这有助于建设零废物城市。以SULM作为类芬顿催化剂,通过界面和溶液协同效应实现了对有机污染物的高效降解过程。在我们的SULM + NHOH + H₂O类芬顿体系中,NHOH能够有效促进界面铁(Fe(Ⅲ)/Fe(Ⅱ))和溶液铁(Fe(Ⅲ)/Fe(Ⅱ))的氧化还原循环,从而促进活性氧物种(ROS)的生成。然而,NHOH存在时ROS的生成过程以及有机污染物的降解途径仍是一个谜。在此,基于实验探索和表征,详细阐述了ROS的生成机制和污染物的降解途径。其中,羟基自由基(·OH)和单线态氧(¹O₂)是氧化和降解有机污染物的主要ROS。值得注意的是,在SULM + NHOH + H₂O体系中,¹O₂可由超氧自由基(·O₂⁻)转化而来。本研究不仅展示了“变废为宝”和“以废治废”的策略,以同时减少工业固体废物和有机废水中的有害排放,还为NHOH介导的类芬顿氧化还原体系提供了新的机理见解。

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