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一步合成具有增强过硫酸盐催化活性的天然蒙脱石/赤铁矿复合材料用于磺胺甲恶唑降解:效率、动力学及机理

One-step synthesis of natural montmorillonite/hematite composites with enhanced persulfate catalytic activity for sulfamethoxazole degradation: Efficiency, kinetics, and mechanism.

作者信息

He Peng, Xiong Yao, Chen Yaozong, Liu Mengfei, Zhu Jianyu, Gan Min

机构信息

School of Minerals Processing and Bioengineering, Key Laboratory of Biohydrometallurgy of Ministry of Education, Central South University, Changsha, 410083, China.

School of Minerals Processing and Bioengineering, Key Laboratory of Biohydrometallurgy of Ministry of Education, Central South University, Changsha, 410083, China.

出版信息

Environ Res. 2022 Mar;204(Pt C):112326. doi: 10.1016/j.envres.2021.112326. Epub 2021 Nov 5.

Abstract

Along with rapid development of sulfate radicals-based advanced oxidation process, efficient, alternatively eco-friendly and cost-effective catalyst is of uppermost priority. However, expensive chemicals are used as source of metal in most of these catalysts, and lose sight of the abundant natural mineral resources on immediate surroundings. In this work, montmorillonite and hematite, two of abundantly natural minerals were utilized to prepare a persulfate catalyst (TMH@M) for sulfamethoxazole (SMX) degradation. The results indicated more than 91% of SMX was removed within 60 min in TMH@M/PS system. The degradation efficiency of SMX of TMH@M/PS combined system was impacted by SMX concentration, PS dosage and natural organic matters, and can remain stable in a certain concentration of HA/chelating agent and a wide pH range (3.01-9.06). Radical scavenging and EPR tests demonstrated O, OH, and SO were major reactive oxygen species in the TMH@M/PS system, while the latter seems more important for degradation of SMX. The results of SEM-EDS, XRD and XPS conformed that low valence iron species (Fe, Fe and FeO) on TMH@M surface are the main driving force behind PS activation to generate reactive species. Furthermore, the iron species on TMH@M surface were transformed during reaction, that in favor of mitigating metal leaching. This work presented a method based on ubiquitous natural minerals to prepare catalyst with excellent PS activate performance for organic wastewater treatment implying a new strategy in minerals utilization deeply and a promisingly alternative process for organic wastewater treatment based on mineral materials.

摘要

随着基于硫酸根自由基的高级氧化工艺的快速发展,高效、环保且具有成本效益的催化剂成为当务之急。然而,这些催化剂大多使用昂贵的化学品作为金属源,而忽视了周围丰富的天然矿产资源。在这项工作中,利用蒙脱石和赤铁矿这两种丰富的天然矿物制备了一种用于磺胺甲恶唑(SMX)降解的过硫酸盐催化剂(TMH@M)。结果表明,在TMH@M/PS体系中,60分钟内SMX的去除率超过91%。TMH@M/PS组合体系对SMX的降解效率受SMX浓度、PS用量和天然有机物的影响,并且在一定浓度的HA/螯合剂和较宽的pH范围(3.01-9.06)内能够保持稳定。自由基清除和EPR测试表明,O、OH和SO是TMH@M/PS体系中的主要活性氧物种,而后者对SMX的降解似乎更为重要。SEM-EDS、XRD和XPS的结果证实,TMH@M表面的低价铁物种(Fe、Fe和FeO)是PS活化产生活性物种的主要驱动力。此外,TMH@M表面的铁物种在反应过程中发生了转化,这有利于减轻金属浸出。这项工作提出了一种基于普遍存在的天然矿物制备具有优异PS活化性能的催化剂用于有机废水处理的方法,这意味着在矿物利用方面有了一种新策略,并且是一种基于矿物材料的有机废水处理的有前景的替代工艺。

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