Rape Straw Supported FeS Nanoparticles with Encapsulated Structure as Peroxymonosulfate and Hydrogen Peroxide Activators for Enhanced Oxytetracycline Degradation

Iron-based catalysts with high load content of iron sulfide (FeS) were commonly peroxymonosulfate (PMS) and hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) activators to degrade organic pollutants but limited catalytic efficiency and increased risk of ferrous ion leaching rest...

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Main Authors: Guiyin Wang, Yan Yang, Xiaoxun Xu, Shirong Zhang, Zhanbiao Yang, Zhang Cheng, Junren Xian, Ting Li, Yulin Pu, Wei Zhou, Gang Xiang, Zhien Pu
Format: Article
Language:English
Published: MDPI AG 2023-03-01
Series:Molecules
Subjects:
Online Access:https://www.mdpi.com/1420-3049/28/6/2771
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author Guiyin Wang
Yan Yang
Xiaoxun Xu
Shirong Zhang
Zhanbiao Yang
Zhang Cheng
Junren Xian
Ting Li
Yulin Pu
Wei Zhou
Gang Xiang
Zhien Pu
author_facet Guiyin Wang
Yan Yang
Xiaoxun Xu
Shirong Zhang
Zhanbiao Yang
Zhang Cheng
Junren Xian
Ting Li
Yulin Pu
Wei Zhou
Gang Xiang
Zhien Pu
author_sort Guiyin Wang
collection DOAJ
description Iron-based catalysts with high load content of iron sulfide (FeS) were commonly peroxymonosulfate (PMS) and hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) activators to degrade organic pollutants but limited catalytic efficiency and increased risk of ferrous ion leaching restricted their use. Meanwhile, various biomass materials such as straw, peel, and branch have been extensively prepared into biochar for mechanical support for iron-based catalysts; however, the preparation process of biochar was energy-intensive. In this study, FeS nanoparticles modified rape straw composites (RS–FeS) encapsulated with ethylenediaminetetraacetic acid (RS–EDTA–FeS) were successfully presented by in-situ synthesis method for efficiently activating PMS and H<sub>2</sub>O<sub>2</sub> to degrade oxytetracycline (OTC), which was economical and environmentally friendly. The results showed that the modified rape straw can remove OTC efficiently, and the addition of EDTA also significantly enhanced the stability and the reusability of the catalyst. In addition, EDTA also promoted the activation of H<sub>2</sub>O<sub>2</sub> at neutral pH. The OTC degradation efficiency of the two catalysts by PMS was faster than that of H<sub>2</sub>O<sub>2</sub>, but H<sub>2</sub>O<sub>2</sub> had a stronger ability to remove OTC than PMS. The highest OTC removal efficiency of RS–FeS and RS–EDTA–FeS were 87.51 and 81.15%. O<sub>2</sub><sup>•–</sup> and <sup>1</sup>O<sub>2</sub> were the major reactive oxidative species (ROS) in the PMS system. Furthermore, compared with RS–FeS, the addition of EDTA inhabited the generation of O<sub>2</sub><sup>•–</sup> in the PMS system. Instead, O<sub>2</sub><sup>•–</sup> and <sup>•</sup>OH were the major ROS in the H<sub>2</sub>O<sub>2</sub> system, but <sup>1</sup>O<sub>2</sub> was also identified in RS–FeS/H<sub>2</sub>O<sub>2</sub> system. RS–EDTA–FeS showed a trend of rising first and then decreasing in recycle test. Instead, the removal rate of OTC by RS–FeS decreased significantly with the increase in reuse times. In the actual wastewater test, the TOC removal of two catalysts active by H<sub>2</sub>O<sub>2</sub> was better than PMS, which was consistent with the test results of OTC, indicating that the two catalysts have application value in the removal of organic pollutants in actual wastewater. This study directly used plant materials as catalysts and omits the preparation process of biochar, greatly reduces the preparation cost and secondary pollution of catalysts, and provides theoretical support for the deepening of advanced oxidation technology.
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spelling doaj.art-b535db265a0e46b282edca766455a2482023-11-17T12:54:58ZengMDPI AGMolecules1420-30492023-03-01286277110.3390/molecules28062771Rape Straw Supported FeS Nanoparticles with Encapsulated Structure as Peroxymonosulfate and Hydrogen Peroxide Activators for Enhanced Oxytetracycline DegradationGuiyin Wang0Yan Yang1Xiaoxun Xu2Shirong Zhang3Zhanbiao Yang4Zhang Cheng5Junren Xian6Ting Li7Yulin Pu8Wei Zhou9Gang Xiang10Zhien Pu11College of Environmental Sciences, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Environmental Sciences, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Environmental Sciences, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Environmental Sciences, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Environmental Sciences, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Environmental Sciences, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Environmental Sciences, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Resources, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Resources, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Resources, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Agronomy, Sichuan Agricultural University, Chengdu 611130, ChinaCollege of Agronomy, Sichuan Agricultural University, Chengdu 611130, ChinaIron-based catalysts with high load content of iron sulfide (FeS) were commonly peroxymonosulfate (PMS) and hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) activators to degrade organic pollutants but limited catalytic efficiency and increased risk of ferrous ion leaching restricted their use. Meanwhile, various biomass materials such as straw, peel, and branch have been extensively prepared into biochar for mechanical support for iron-based catalysts; however, the preparation process of biochar was energy-intensive. In this study, FeS nanoparticles modified rape straw composites (RS–FeS) encapsulated with ethylenediaminetetraacetic acid (RS–EDTA–FeS) were successfully presented by in-situ synthesis method for efficiently activating PMS and H<sub>2</sub>O<sub>2</sub> to degrade oxytetracycline (OTC), which was economical and environmentally friendly. The results showed that the modified rape straw can remove OTC efficiently, and the addition of EDTA also significantly enhanced the stability and the reusability of the catalyst. In addition, EDTA also promoted the activation of H<sub>2</sub>O<sub>2</sub> at neutral pH. The OTC degradation efficiency of the two catalysts by PMS was faster than that of H<sub>2</sub>O<sub>2</sub>, but H<sub>2</sub>O<sub>2</sub> had a stronger ability to remove OTC than PMS. The highest OTC removal efficiency of RS–FeS and RS–EDTA–FeS were 87.51 and 81.15%. O<sub>2</sub><sup>•–</sup> and <sup>1</sup>O<sub>2</sub> were the major reactive oxidative species (ROS) in the PMS system. Furthermore, compared with RS–FeS, the addition of EDTA inhabited the generation of O<sub>2</sub><sup>•–</sup> in the PMS system. Instead, O<sub>2</sub><sup>•–</sup> and <sup>•</sup>OH were the major ROS in the H<sub>2</sub>O<sub>2</sub> system, but <sup>1</sup>O<sub>2</sub> was also identified in RS–FeS/H<sub>2</sub>O<sub>2</sub> system. RS–EDTA–FeS showed a trend of rising first and then decreasing in recycle test. Instead, the removal rate of OTC by RS–FeS decreased significantly with the increase in reuse times. In the actual wastewater test, the TOC removal of two catalysts active by H<sub>2</sub>O<sub>2</sub> was better than PMS, which was consistent with the test results of OTC, indicating that the two catalysts have application value in the removal of organic pollutants in actual wastewater. This study directly used plant materials as catalysts and omits the preparation process of biochar, greatly reduces the preparation cost and secondary pollution of catalysts, and provides theoretical support for the deepening of advanced oxidation technology.https://www.mdpi.com/1420-3049/28/6/2771organic pollutantsadvanced oxidationfenton/fenton-like processsinglet oxygenwastewater treatment
spellingShingle Guiyin Wang
Yan Yang
Xiaoxun Xu
Shirong Zhang
Zhanbiao Yang
Zhang Cheng
Junren Xian
Ting Li
Yulin Pu
Wei Zhou
Gang Xiang
Zhien Pu
Rape Straw Supported FeS Nanoparticles with Encapsulated Structure as Peroxymonosulfate and Hydrogen Peroxide Activators for Enhanced Oxytetracycline Degradation
Molecules
organic pollutants
advanced oxidation
fenton/fenton-like process
singlet oxygen
wastewater treatment
title Rape Straw Supported FeS Nanoparticles with Encapsulated Structure as Peroxymonosulfate and Hydrogen Peroxide Activators for Enhanced Oxytetracycline Degradation
title_full Rape Straw Supported FeS Nanoparticles with Encapsulated Structure as Peroxymonosulfate and Hydrogen Peroxide Activators for Enhanced Oxytetracycline Degradation
title_fullStr Rape Straw Supported FeS Nanoparticles with Encapsulated Structure as Peroxymonosulfate and Hydrogen Peroxide Activators for Enhanced Oxytetracycline Degradation
title_full_unstemmed Rape Straw Supported FeS Nanoparticles with Encapsulated Structure as Peroxymonosulfate and Hydrogen Peroxide Activators for Enhanced Oxytetracycline Degradation
title_short Rape Straw Supported FeS Nanoparticles with Encapsulated Structure as Peroxymonosulfate and Hydrogen Peroxide Activators for Enhanced Oxytetracycline Degradation
title_sort rape straw supported fes nanoparticles with encapsulated structure as peroxymonosulfate and hydrogen peroxide activators for enhanced oxytetracycline degradation
topic organic pollutants
advanced oxidation
fenton/fenton-like process
singlet oxygen
wastewater treatment
url https://www.mdpi.com/1420-3049/28/6/2771
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