Sulfadiazine removal by peroxymonosulfate activation with sulfide-modified microscale zero-valent iron: Major radicals, the role of sulfur species, and particle size effect

Ling, Chen; Wu, Shuai; Dong, Tailu; Dong, Haifan; Wang, Zhengxiao; Pan, Yuwei; Han, Jun

doi:10.1016/j.jhazmat.2021.127082

Cited by 62 publications

(12 citation statements)

References 54 publications

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“…The most recent work on liquid precipitation method for SZVI preparation is a multireaction system and usually contains a step of Fe(II) release before it reacts with the sulfur source (Na 2 S). ,– In this case, there are three potential pathways for FeS x formation on the ZVI surface through the bonded FeS x /Fe interface: (a) reaction of inherent iron-containing compounds on the ZVI surface with S(–II), – (b) in situ formation of FeS x by surface-generated Fe(II) with S(–II), – and (c) precipitation of externally formed FeS x solid on the ZVI surface. , However, the interfacial reaction of Fe 0 , Fe(II), S(–II), and FeS x on the ZVI surface is still not clear. In order to investigate the decisive pathway of forming the FeS x /Fe interface, three different systems for the preparation of SZVI were designed to simulate the above pathways by controlling the Fe(II) source and location (Scheme ), thus probing the real interface-exchange process.…”

Section: Resultsmentioning

confidence: 99%

“…The construction of the FeS x -containing ZVI structure can be achieved through several well-developed strategies, among which the mechanical ball-milling method undergoes a direct reaction of Fe 0 and S 0 (solid–solid reaction) to form the surface FeS x , – while the liquid precipitation method (solid–liquid reaction) undergoes a complex physical and chemical process. However, the complexity of the solid–liquid reaction makes it unclear how the FeS x /Fe interface is formed. ,, The formation of FeS x is the prerequisite of SZVI preparation by the liquid precipitation method, and in this method, the commonly used sulfur sources are Na 2 S 2 O 4 , Na 2 S 2 O 3 , and Na 2 S. Although the process of FeS x formation from these sulfur sources is different, these sulfur sources can become S(–II) through the reactions of decomposition, hydrolysis, and disproportionation, and finally, S(–II) acts as the direct sulfur precursor that reacts with Fe(II) to form FeS x . , Unlike S(–II) that is produced in the liquid phase, the Fe(II) precursor comes from the release of iron ions from the solid phase, as a consequence of the oxidation of ZVI. ,– As the chemical state of Fe(II) has a significant impact on FeS x formation, whether the Fe(II) precursor produced from the solid ZVI is adsorbed on the surface or released into the solution is an important factor in the formation of surface FeS x during SZVI preparation.…”

Section: Introductionmentioning

confidence: 99%

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Chemical Bond Bridging across Two Domains: Generation of Fe(II) and In Situ Formation of FeS_x on Zerovalent Iron

Zhang

Duan

Jin

et al. 2023

Environ. Sci. Technol.

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Sulfidation of zerovalent iron (SZVI) can strengthen the decontamination ability by promoting the electron transfer from inner Fe0 to external pollutants by iron sulfide (FeS x ). Although FeS x forms easily, the mechanism for the FeS x bonding on the ZVI surface through a liquid precipitation method is elusive. In this work, we demonstrate a key pathway for the sulfidation of ZVI, namely, the in situ formation of FeS x on ZVI surface, which leads to chemical bonding across two domains: the pristine ZVI and the newly formed FeS x phase. The two chemically bridged heterophases display superior activity in electron transportation compared to the physically coated SZVI, eventually bringing about the better performance in reducing Cr(VI) species. It is revealed that the formation of chemically bonded FeS x requires balancing the rates for the two processes of Fe(II) release and sulfidation, which can be achieved by tuning the pH and S(–II) concentration. This study elucidates a mechanism for surface generation of FeS x on ZVI, and it provides new perspectives to design high-quality SZVI for environmental applications.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Chemical Bond Bridging across Two Domains: Generation of Fe(II) and In Situ Formation of FeS_x on Zerovalent Iron

Zhang

Duan

Jin

et al. 2023

Environ. Sci. Technol.

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“…9(a), for original Fe 3 O 4 @FeEDTA, the spectrum of Fe 2p3/2 on the surface of Fe 3 O 4 @FeEDTA could be deconvoluted into three peaks at 709.7, 710.8 eV and 713.2 eV. The two peaks at 709.7 and 713.2 eV correspond to Fe(II) and Fe(III) of oxidized species, 47 which may be formed by the superficial oxidation of Fe upon exposure to air. The peak at 710.8 eV (Fe 2p3/2) demonstrated the existence of FeN bonding, 48 which further proved that the FeEDTA was successfully loaded onto Fe 3 O 4 .…”

Section: Resultsmentioning

confidence: 99%

“…The two peaks at 709.7 and 713.2 eV correspond to Fe(II) and Fe(III) of oxidized species, 47 which may be formed by the superficial oxidation of Fe upon exposure to air. The peak at 710.8 eV (Fe 2p3/2) demonstrated the existence of Fe N bonding, 48 which further proved that the FeEDTA was successfully loaded onto Fe 3 O 4 .…”

Section: Reaction Mechanismmentioning

confidence: 99%

Effective nitric oxide removal from flue gas using UV/H₂O₂ solution catalyzed by Fe₃O₄@FeEDTA

Liu

Zhou

et al. 2023

J of Chemical Tech & Biotech

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BACKGROUND: How to control NO x emission in flue gas economically and efficiently is the focus in the field of energy and environment in the world. In this work, Fe 3 O 4 -magnetic microspheres were employed as the matrix with loading FeEDTA (where EDTA is ethylenediaminetetraacetic acid) to prepare magnetic denitrification absorbent Fe 3 O 4 @FeEDTA. The performance of nitric oxide (NO) removal using Fe 3 O 4 @FeEDTA dispersed in H 2 O 2 solution with ultraviolet (UV) was first investigated. RESULTS:The results showed that Fe 3 O 4 @FeEDTA could be used as a good catalytic oxidation denitrification agent. Increasing H 2 O 2 concentration and O 2 concentration could promote NO absorption. NO removal efficiency increased as pH value increased from 1.5 to 3.0, then decreased when pH continued to increase. The elevated temperature was conducive to NO removal. CO 2 hardly affected the removal of NO, while SO 2 with high concentration was not conducive to NO absorption. In addition, the NO removal mechanism was preliminarily analyzed with X-ray photoelectron spectrometry, electron spin resonance and ion chromatography. The mechanism study indicated that NO removal by Fe 3 O 4 @FeEDTA/H 2 O 2 was a catalysis-complexation-oxidation-absorption process, in which •OH was determined to be the main oxidizing species, and NO captured by Fe(II)EDTA was mainly oxidized by •OH to NO 3 − . CONCLUSION: The catalytic activity of Fe 3 O 4 @FeEDTA could maintain stability during the repeat experiment, realizing the recycling and reuse of Fe 3 O 4 @FeEDTA. The UV-Fe 3 O 4 @FeEDTA-activated H 2 O 2 advanced oxidation technology is suitable for wet denitrification.

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“…RS–FeS improved the degradation of OTC by PMS or H 2 O 2 , more than 80.00% of OTC was removed within 30.00 min. This proved that dispersing FeS onto the surface of RS is an efficient way to enhance the catalytic performance of RS [ 49 ]. In addition, OTC was also efficiently removed by FeS within 30 min, indicating that FeS exhibited facilitation in activating PMS and H 2 O 2 .…”

Section: Resultsmentioning

confidence: 99%

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

Wang

Yang

et al. 2023

Molecules

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Iron-based catalysts with high load content of iron sulfide (FeS) were commonly peroxymonosulfate (PMS) and hydrogen peroxide (H2O2) 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 H2O2 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 H2O2 at neutral pH. The OTC degradation efficiency of the two catalysts by PMS was faster than that of H2O2, but H2O2 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%. O2•– and 1O2 were the major reactive oxidative species (ROS) in the PMS system. Furthermore, compared with RS–FeS, the addition of EDTA inhabited the generation of O2•– in the PMS system. Instead, O2•– and •OH were the major ROS in the H2O2 system, but 1O2 was also identified in RS–FeS/H2O2 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 H2O2 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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Sulfadiazine removal by peroxymonosulfate activation with sulfide-modified microscale zero-valent iron: Major radicals, the role of sulfur species, and particle size effect

Cited by 62 publications

References 54 publications

Chemical Bond Bridging across Two Domains: Generation of Fe(II) and In Situ Formation of FeS_x on Zerovalent Iron

Chemical Bond Bridging across Two Domains: Generation of Fe(II) and In Situ Formation of FeS_x on Zerovalent Iron

Effective nitric oxide removal from flue gas using UV/H₂O₂ solution catalyzed by Fe₃O₄@FeEDTA

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

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Sulfadiazine removal by peroxymonosulfate activation with sulfide-modified microscale zero-valent iron: Major radicals, the role of sulfur species, and particle size effect

Cited by 62 publications

References 54 publications

Chemical Bond Bridging across Two Domains: Generation of Fe(II) and In Situ Formation of FeSx on Zerovalent Iron

Chemical Bond Bridging across Two Domains: Generation of Fe(II) and In Situ Formation of FeSx on Zerovalent Iron

Effective nitric oxide removal from flue gas using UV/H2O2 solution catalyzed by Fe3O4@FeEDTA

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

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Chemical Bond Bridging across Two Domains: Generation of Fe(II) and In Situ Formation of FeS_x on Zerovalent Iron

Chemical Bond Bridging across Two Domains: Generation of Fe(II) and In Situ Formation of FeS_x on Zerovalent Iron

Effective nitric oxide removal from flue gas using UV/H₂O₂ solution catalyzed by Fe₃O₄@FeEDTA