ENVIRONMENTAL RESEARCH
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2023
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IF 8.3
Wen Qin,Jianshan Peng,Jingru Yang,Yang Song,Jun Ma
In this study, the relative residual UV absorbance (UV 254 ) and/or electron donating capacity (EDC) was investigated as a surrogate parameter to evaluate the abatement of micropollutants during the Fe(II)/PMS and Mn(II)/NTA/PMS processes. In the Fe(II)/PMS process, due to the generation of SO 4 •- and •OH at acidic pH, UV 254 and EDC abatement was greater at pH 5. In the Mn(II)/NTA/PMS process, UV 254 abatement was greater at pH 7 and 9, while EDC abatement was greater at pH 5 and 7. This was attributed to the fact that MnO 2 was formed at alkaline pH to remove UV 254 by coagulation, and manganese intermediates (Mn(V)) were formed at acidic pH to remove EDC via electron transfer . Due to the strong oxidation capacity of SO 4 •- , •OH and Mn(V), the abatement of micropollutants increased with increasing dosages of oxidant in different waters in both processes. In the Fe(II)/PMS and Mn(II)/NTA/PMS processes, except for nitrobenzene (∼23% and 40%, respectively), the removal of other micropollutants was greater than 70% when the oxidant dosages were greater in different waters. The linear relationship between the relative residual UV 254 , EDC and the removal of micropollutants was established in different waters, showing a one-phase or two-phase linear relationship. The differences of the slopes for one-phase linear correlation in the Fe(II)/PMS process (micropollutant-UV 254 : 0.36–2.89, micropollutant-EDC: 0.26–1.75) were less than that in the Mn(II)/NTA/PMS process (micropollutant-UV 254 : 0.40–13.16, micropollutant-EDC: 0.51–8.39). Overall, these results suggest that the relative residual UV 254 and EDC could truly reflect the removal of micropollutants during the Fe(II)/PMS and Mn(II)/NTA/PMS processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Zhengyuan Zhou,Jingyao Huang,Zhiqiang Xu,Meesam Ali,Ali Shan,Rongbing Fu,Shuguang Lyu
In this study, trichloroethene (TCE) removal was remarkably enhanced with the addition of Fe(II)/CA (citric acid), Fe(II)/nZVI (nano zero-valent iron) and Fe(II)/S-nZVI (sulfidated nano zero-valent iron), respectively, as synergistic activated catalysts in persulfate environment. Among them, the better performance of TCE removal followed the order of PS/Fe(II)/S-nZVI > PS/Fe(II)/nZVI > PS/Fe(II)/CA ≫ PS/Fe(II), and the majority of TCE was declorinated to Cl − . The scavenger and EPR tests indicated that HO and SO 4 − were responsible for TCE degradation. Further study was conducted through the calculation of reaction rate constants, demonstrating HO produced from SO 4 − was of greater significance than SO 4 − itself. With the presence of CA , the concentration of Fe(II) was maintained at a desired level to proceed the catalytic activity. Meanwhile, S-nZVI and nZVI had ability to convert Fe(III) to Fe(II), and sulfur species, especially S(-II) in S-nZVI acted as an reductant to a certain extent. Sufficient Fe(II) in solution activated PS to produce adequate HO for TCE degradation. Furthermore, the broad-spectrum reactivity in different systems were investigated, and the results indicated that most of the chloroalkenes and benzene series frequently detected in contaminated sites could also be removed at the desired chemicals ratio. In conclusion, this research revealed the superiority of synergistic activated catalysts and provided theoretical bases for the remediation of TCE and other pollutants in actual contaminated groundwater.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Runliang Zhu,Yanping Zhu,Haiyang Xian,Lixia Yan,Haoyang Fu,Gangqiang Zhu,Yunfei Xi,Jianxi Zhu,Hongping He
The generation of Fe(II) from Fe(III) is the rate-limiting step in the heterogeneous Fenton reaction, and accelerating this step is critical for enhancing the reaction efficiency and also the subject of extensive studies. In this work, the oxidized multi-walled carbon nanotubes (CNTs) were coupled with ferrihydrite (Fh) to synthesize novel and highly efficient heterogeneous Fenton catalysts (CNTs/Fh). Interestingly, the calculated apparent rate constants by 3%CNTs/Fh could reach ∼7.1 times as high as that by Fh, well in agreement with the accelerated decomposition rate of H 2 O 2 , as well as the enhanced generation rate of Fe(II) and hydroxyl radicals in the CNTs/Fh system. The density functional theory calculations and the cyclic voltammograms curves both well indicated that the Fe(III)/Fe(II) redox cycling on CNTs/Fh could be significantly enhanced during the Fenton reaction, from both dynamic (accelerating the electron transfer from H 2 O 2 to Fh) and thermodynamic (lowering Fe(III)/Fe(II) redox potential) aspects.
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FOOD CHEMISTRY
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2019
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IF 5.399
Yuelin Kong,Qiao Cheng,Yu He,Yili Ge,Jiangang Zhou,Gongwu Song
A fluorometric and colorimetric dual-mode sensing platform based on graphitic carbon nitrite quantum dots (g-CNQDs) and Fe (II)-bathophenanthroline complex (BPS-Fe 2+ ) was designed to the sensitive detection of nitrite (NO 2 − ) in sausage and water. In this system, the fluorescence of g-CNQDs was quenched by BPS-Fe 2+ complex due to the inner filter effect (IFE). When NO 2 − was present, Fe 2+ was oxidized by nitrite to form BPS-Fe 3+ complex with BPS, leading to the recovery of the fluorescence from g-CNQDs. Therefore, we constructed a “turn-off-on” fluorescence probe for detection of NO 2 − . Moreover, with the increase of NO 2 − concentration, the color of the solution changed from red to colorless, so the UV–vis measurements and on-site visual detection were realized. The method is capable of detecting NO 2 − in the concentration range of 2.32–34.8 μM with good selectivity and high sensitivity. In addition, the method has the potential to determine NO 2 − in water samples and sausage samples.
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ENVIRONMENTAL POLLUTION
·
2024
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IF 7.6
Chen Wu,Sicheng Hang,Feng Li,Yujun Wu,Shengwei Yi,Xingang Liu,Mingjie Chen,Fei Ge,Jiang Tian,Ming Zhang,Dayi Zhang
Rice rhizosphere soil-porewater microdomains exist within an iron (Fe)-rich microoxic habitat during paddy soil flooding. However, the response mechanisms of core microflora in this habitat to Fe(II)-oxidation-mediated cadmium (Cd) and phenanthrene (Phen) remain unclear. Using gel-stabilized gradient systems to replicate the microoxic conditions in the rice rhizosphere porewater, we found that microaerophilic rhizobacteria drove Fe(II) oxidation to yield iron oxides, thereby reducing the Cd and Phen contents in the rhizosphere porewater and rice (Cd and Phen decreased by 15.9%–78.0% and 10.1%–37.4%, respectively). However, co-exposure to Cd and Phen resulted in a greater reduction in the Cd uptake and a greater increase in the Phen uptake in rice as compared to those in the Cd or Phen treatments, possibly attributing to the cation-π interactions between Cd and Phen, as well as competition between the adsorption sites on the roots. The elevation of Cd-tolerant genes and Phen-degradation genes in biogenic cell-mineral aggregates unveiled the survival strategies of rhizobacteria with respect to Cd and Phen in the microoxic habitat. Potential Cd-tolerant rhizobacteria (e.g., Pandoraea and Comamonas ) and Phen-degradation rhizobacteria (e.g., Pseudoxanthobacter ) were identified through the DNA-SIP and 16S rRNA gene amplicon sequencing. Metagenomic analysis further confirmed that these core microbes harbor Cd-tolerant, Phen-degradation, and Fe(II) oxidation genes, supporting their metabolic potential for Cd and/or Phen in the microoxic habitat of the rice rhizosphere. These findings suggest the potential mechanism and ecological significance of core rhizospheric microbial-driven Fe(II) oxidation in mitigating the bioavailability of Cd and Phen in paddy soil during flooding.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Zhongmou Liu,Pan Zhang,Xiangyu Zhao
Reduced graphene oxide supported with ferric ion (Fe(III)-rGO) was successfully prepared, and performed as an excellent catalyst to activate hydrogen peroxide (H 2 O 2 ) and peroxymonosulfate (PMS) for isoprothiolane (IPT) degradation. IPT removal efficiency was proven to be better in the Fe(III)-rGO/H 2 O 2 /PMS system (96.2%) than in the Fenton-like reaction (72.6%) and PMS-AOP (80.0%) individually. X-ray photoelectron spectroscopy showed that Fe(III) was reduced in Fenton-like reaction, and the reduced Fe(II) played a crucial role in the subsequent PMS-AOP. The combination of the Fenton-like reaction and PMS-AOP involved the valence state conversion of Fe, which consequently improved Fe(III)-rGO utilization rate and IPT removal efficiency. Fe(III)-rGO remarkably boosted the Fe(III)/Fe(II) cycle and generated superoxide radical (O 2 − •) and singlet oxygen ( 1 O 2 ) in the Fe(III)-rGO/H 2 O 2 /PMS system. Fe(III)-rGO acts as the electron transfer mediator; thus, promoting electron transfer from IPT to H 2 O 2 and PMS and accelerating the generation of active species. Fe(IV) with high oxidation performance was formed in PMS-AOP and efficiently removed some of the IPT. IPT removal efficiency was more than 90% at a pH range of 3–11; this efficiency could be maintained above 50% even after five consecutive degradation experiments, exhibiting excellent stability and reusability of Fe(III)-rGO. Additionally, iron sludge formation was greatly reduced because of the stable chemical bonding of iron ions to the rGO surface. Therefore, this study provides a new multisystem and synergistic approach for the efficient removal of organic micro-pollutants from water.
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CHEMOSPHERE
·
2024
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IF 8.1
Jie Zhang,Xufei Wang,Yiwei Liu,Tao Jin,Liang Liu,Xiaodong Ma,Gengbo Ren
The efficiency and stability of the electrical activation of persulfate (PS) by transition metal-based cathode are controlled by the cycling of Fe(III)/Fe(II) and the mass transfer of PS. In this study, the mixed-valence MOFs catalyst (Fe II -MIL-53(Fe)) modified flow-through cathode was prepared for the first time. Fe II -MIL-53(Fe) was prepared by replacing part of the iron-oxygen network structure in MIL-53(Fe) with Fe(II), resulting in the formation of coordinated unsaturated iron centers (CUICs). The increase of the Fe(III) CUICs facilitated the conversion of Fe(III) to Fe(II). Furthermore, the cycling of Fe(III)/Fe(II) was further promoted by the electric field. Meanwhile, the hydrodynamic behavior of flow-through cathode was indicated by the computational fluid dynamics (CFD) simulation. The quenching experiments and electron paramagnetic resonance (EPR) results showed that several reactive specie (SO 4 ·- , ·OH, O 2 ·- and 1 O 2 ) were produce. In summary, this work provided an effective strategy for the efficient and stable electrical activation of PDS.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Rong Li,Yiziqi Lu,Meiqian Lu,Yue Liu,Guodong Zhang,Qiuling Ma,Jian Zhou,Tiecheng Wang
Iodinated X-ray contrast media, as a frequently used medical diagnosis in the imaging of internal organs, soft tissues, and blood vessels, are widely encountered in water environments because of their non-metabolic ability. Herein, a series of co-precipitates (DBC-FeO x ) of dissolved black carbon (DBC) and FeO x were successfully synthesized. The chelation of Fe species with COO – groups in DBC enhanced the excellent electron transfer capability and persulfate (PS) activation performance of the resulting DBC-FeO x , thus boosting iopamidol (IPM) degradation. The IPM removal rate constant in the DBC-FeO x /PS was 35 times and 4.6 times higher than those observed in the DBC/PS and FeO x /PS systems, respectively. There existed an appropriate C/Fe molar ratio in the DBC-FeO x co-precipitates for PS activation, and the IPM degradation was driven by both radical and non-radical pathways. Fe sites were the primary active sites in DBC-FeO x for PS activation, and C=O groups played an important role in accelerating the Fe(III)/Fe(II) cycle by promoting rapid electron transfer, thereby enhancing radical oxidation pathways. Concurrently, DBC-FeO x acted as an electron shuttle to promote the electron transfer from IPM to PS, creating non-radical pathways for IPM removal. IPM degradation processes involved amide hydrolysis oxidation, hydrogen extraction, and deiodination. The typical iodine species HOI was also converted to non-toxic IO 3 - after IPM decomposition, thus reducing potential risks.
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CHEMOSPHERE
·
2022
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IF 8.943
Wenkai Liu,Bin Liu,Xin Li
The aim of this study was to investigate the feasibility and fouling mitigation mechanisms of UV/Fe(II) synergistically activated sulfite (S(IV)) (UFS) pretreatment to alleviate membrane fouling caused by HA-enhanced Ca 2+ scaling. After UFS treatment, hydrophobic substances and carboxyl groups structure were destroyed by the in-situ-generated SO•–4, resulted in a significant reduction of hydrophobic substances ratio and carboxyl group concentration. Due to the formation of more electropositive in-situ-generated Fe(III), the complexation between Ca 2+ and carboxyl groups was weakened so that the bulk crystallization size on the membrane surface was greatly reduced. The filter cake enhanced osmotic pressure effect (CEOP) and concentration polarization effect were hence alleviated, as well as the surface roughness . At the microcosmic perspective, as the energy barrier between the membrane and foulants was increased significantly after pretreatment, the anti -foulants adsorption ability of the membrane was enhanced. Correlation analysis showed that the carboxyl concentration and density, HPO ratio, larger particle size (>100 nm) ratio, the Ca 2+ concentration in the scaling layer and energy barrier all had a good correlation with the membrane resistance. This research not only provides an advanced oxidation technology that can effectively alleviate the synergistically-fouling effect of HA and Ca 2+ of nanofiltration process, but also proposes a guidance for the UV/Fe(II) synergistically activated sulfite.
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VACUUM
·
2023
·
IF 4
Chaoqun Yan,Zhiliang Cheng,Xuan Zhang,Juan Wei,Qian Xu
The photocatalytic efficiency of hematite (α-Fe 2 O 3 ) is limited by its photoexcited state lifetime and diffusion length. By adjusting the surface structure, the photogenerated electron pairs can migrate to the surface and the charge recombination can be suppressed, which can effectively solve these problems and improve the photo-Fenton performance. In this study, four kinds different morphologies of α-Fe 2 O 3 - x (truncated hexagonal bipyramidal, cubic, hexagonal shape, and spherical) were synthesized by hydrothermal method , and a photocatalyst (H-α-Fe 2 O 3 - x ) with higher catalytic activity was prepared by hydrogenation. The results of UV–Vis DRS , PL , Raman, and XPS analysis , the oxygen vacancies and Fe (II) species were introduced into the α-Fe 2 O 3 catalyst after the hydrogenation reaction. The H-α-Fe 2 O 3 - x showed good degradation performance for TC and DX as EMPs model pollutants. The results show that the formation of oxygen vacancy and Fe 2+ is the main factor to improve the photocatalytic activity of the reaction system. Furthermore, the reaction mechanism revealed that reactive radicals involved in the H-α-Fe 2 O 3 - x photocatalytic system were •OH, •O 2 − , and h + responsible. This study provides an alternative technology for an easy and effective means for bandgap engineering to improve the photocatalytic performance of photocatalysts and facilitate widening environmental application.
研究领域:
环境科学
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材料科学
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化学
·
光催化
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Qiangshun Wu,Hanpei Yang,Li Kang,Zhao Gao,Feifan Ren
In this work, a series of Fe-based metal-organic frameworks (Fe-MOFs) were synthesized and served as Fenton-like catalysts for tetracycline hydrochloride (TC–HCl) degradation. Herein, for the first time, we have demonstrated that visible light can accelerate Fe(II)/Fe(III) cycle in the photo-Fenton system based on iron-oxo (Fe-O) clusters in frameworks. Among these Fe-MOFs, MIL-101 possessed the highest activity mainly ascribed to its largest specific surface area and pore volume, and the most coordinatively unsaturated iron sites. The synergistic effect in the MIL-101/H 2 O 2 /visible light system was derived from the efficient separation and migration of photogenerated carriers. Due to the function of solid acid catalysts, MIL-101 extended effective pH range up to 10.2 and exhibited good reusability and stability. Hydroxyl radicals generated from H 2 O 2 coordinated at iron active sites were determined as the main reactive oxidative species and acceleration of Fe(II)/Fe(III) cycle was responsible for highly effective degradation of TC–HCl.
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CHEMOSPHERE
·
2025
·
IF 8.1
Qianying Zong,Xiaofei Niu,Xin Cheng,Yifan Liu,Cong Liu,Tingyue Shi,Jiapeng Liu,Xiaohong Yang,Wentao Wang,Zikuan Guo,Fengjuan Xiao
Nanoscale FeWO 4 /BiVO 4 heterojunctions were directly grown on the graphite fiber felt (GF) with good conductivity to construct a FeWO 4 /BiVO 4 @GF solar photo-Fenton like wastewater treatment system. The removal effect of COD from phenolic wastewater and the mechanism of synergistic improvement of wastewater treatment efficiency by this system were investigated. The FeWO 4 /BiVO 4 heterojunction prepared by hydrothermal method exhibited higher photoelectric conversion efficiency and solar light utilization rate, thus endowing FeWO 4 /BiVO 4 with excellent solar-Fenton like reaction activity.The photo-Fenton activity can be maintained well even within the pH range of 2–8. Loading FeWO 4 /BiVO 4 nano-heterojunction on GF helped to increase the contact area between Fenton reagents and wastewater, facilitate the electron transfer on the FeWO 4 /BiVO 4 heterojunction and enable the recovery and reuse of the Fenton reagents.Under solar light radiation, the COD removal efficiency of FeWO 4 /BiVO 4 @GF/H 2 O 2 system in phenolic wastewater was more than 92%. Even after five cycles, the system still exhibited excellent operation stability. FeWO 4 /BiVO 4 @GF promoted the conversion and cycling of Fe(III)/Fe(II) by accelerating the separation and transport of photogenerated electrons/holes and increasing the concentration of active species, thereby stimulating excellent solar photo-Fenton like activity.The results are significance to the development of green and efficient photo-Fenton process for advanced treatment of industrial wastewater.
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