Nanoconfinement-mediated non-radical enhanced pollutant degradation on Fe single-atom electrocatalyst

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Journal of Hazardous Materials Pub Date : 2025-02-26 DOI:10.1016/j.jhazmat.2025.137764
Xinglei Shi , Saixi Chen , Kun Zhao , Shuai Wu , Fei Ye , Hongtao Yu , Yuanhao Zhang , Xiaolong Chen , Yusheng Liang , Junfeng Niu
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Abstract

Heterogeneous electro-Fenton (EF) technology is an efficient approach for antibiotics degradation, but the effective mineralization of pollutants in complex actual water remains challenging due to the susceptibility of hydroxyl radical (∙OH) to environmental influences. Herein, a Fe-single atom anchored porous hollow carbon sphere (FexHCS) material with nano-confinement structure was designed for simultaneously catalyzing H2O2 to produce ∙OH and 1O2. Benefiting from oxidation of ∙OH and selective reaction of alkyl group with 1O2, the kinetic constant (k) of the FexHCS-based EF system achieves 4.13 h−1, which is 3.7 times higher than that of the traditional Fenton (1.13 h−1) under the same conditions for ofloxacin (OFL) degradation. The mineralization efficiency of OFL by FexHCS-based EF reaches 72.7 %, exceeding most of the previously reported catalysts within 1 h. The COD value of actual pharmaceutical wastewater is reduced from 801 mg L−1 to 49 mg L−1 after 5 h of treatment, and the energy consumption for wastewater treatment is calculated to be 15.9 kW h kg−1 COD−1. This work demonstrates the attractive advantages of 1O2 enhanced electro-Fenton performance in complex actual water and provides new insights into developing novel electrocatalysts for wastewater treatment.

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Fe单原子电催化剂纳米束缚介导非自由基强化污染物降解
非均相电fenton (EF)技术是一种有效的抗生素降解方法,但由于羟基自由基(∙OH)对环境影响的敏感性,在复杂的实际水中有效矿化污染物仍然具有挑战性。本文设计了一种具有纳米约束结构的铁单原子锚定多孔空心碳球(FexHCS)材料,用于同时催化H2O2生成∙OH和1O2。得益于∙OH氧化和1O2选择性烷基反应,fexhcs - EF体系在相同条件下降解氧氟沙星(OFL)的动力学常数(k)达到4.13 h-1,是传统Fenton体系(1.13 h-1)的3.7倍。FexHCS-based EF对OFL的矿化效率达到72.7%,在1 h内就超过了大多数已有报道的催化剂。实际制药废水的COD值在处理5 h后由801 mg L-1降至49 mg L-1,计算废水处理能耗为15.9 kW h kg-1 COD-1。这项工作显示了在复杂的实际水中,o2增强电fenton性能的诱人优势,并为开发新型电催化剂用于废水处理提供了新的见解。
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来源期刊
Journal of Hazardous Materials
Journal of Hazardous Materials 工程技术-工程:环境
CiteScore
25.40
自引率
5.90%
发文量
3059
审稿时长
58 days
期刊介绍: The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.
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