MOLECULES
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2019
·Vol. 25
·期 1
·168
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IF 3.06
Chuang Zhang,Haichao Li,Chen Li,Zhengqiang Li
Methods to remove dye pollutants with natural enzyme, like horseradish peroxidase (HRP), are still limited due to high costs and low stability levels. The development of such a method with similar enzymatic activity is important and could be helpful in wastewater disposal. A metal organic framework material, Fe-loaded MOF-545 (Fe), was synthesized in our study as a new way to remove dyes due to its peroxidase-like activity. The structural characterizations of Fe-loaded MOF-545(Fe) was investigated using scanning electron microscopy (SEM), UV-Vis absorption spectra, and X-ray diffraction (XRD). The peroxidase-like (POD-like) activity of Fe-loaded MOF-545(Fe) was investigated under different pH and temperature conditions. Because of the Fe added into the MOF-545 structure, the absorption of Fe-loaded MOF-545(Fe) for acid (anionic) dyes (methyl orange (MO)) was better than for basic (cationic) dyes (methylene blue (MB)). The Fe-loaded MOF-545(Fe) could give a significant color fading for MO and MB over a short time (about two hours) with peroxidase-like activity. The remarkable capacity of Fe-loaded MOF-545(Fe) to remove the MO or MB is due to not only physical adsorption, but also degradation of the MO and MB with POD-like activity. Therefore, Fe-loaded MOF-545(Fe) has significant potential regarding dye removal from wastewater.Keywords:Fe-loaded MOF-545(Fe);peroxidase-like activity;dye absorption;dye degradation;wastewater
研究领域:
材料科学
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环境科学
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生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Maolin Wang,Mi Deng,Gang Zhao,Yanchun Fan,Tianwen Liu,Ying Huang,Lan Peng,Haoyang Fu,Shengqiong Fang
The remediation of organic-contaminated water is a critical environmental challenge, and iron-based persulfate (PS) activation processes have emerged as a promising solution. However, the introduction of reductive sulfur species, while accelerating the Fe(III)/Fe(II) redox cycle, may also quench reactive species, potentially compromising the efficiency of Fenton-like systems. Here we systematically investigate the trade-off between accelerated Fe(III)/Fe(II) cycling and quenching effects in the zerovalent iron/PS (ZVI/PS) system using thiosulfate (TSF) as an activator. Our results show that low-level TSF (0.03–1.00 mmol/L) effectively facilitated the removal of naphthalene (Nap) and atrazine (ATZ), respectively. This enhancement is attributed to accelerated ZVI dissolution and FeS x formation, which promote the Fe(III)/Fe(II) cycle, with Fe(IV) was identified as the primary active species. However, high-level TSF (>1.0 mmol/L) drastically reduced Nap removal due to PS consumption and active species elimination. The optimal TSF dosage of 0.20 mmol/L (TSF/PS molar ratio of 1:10) demonstrated robust organic pollutant degradation, achieving a 22-fold increase in the rate constant ( k obs ) for Nap removal and 0.47–7.5-fold increases for ATZ removal. These findings highlight the potential of the TSF-ZVI/PS system as a versatile and efficient solution for degrading a wide range of organic pollutants, including PAHs and herbicides, in water treatment applications.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
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.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Lina Wang,Hanpei Yang,Li Kang,Mi Wu,Yuankun Yang
In this work, Ag/AgCl/FeOCl (Ag–Fe) catalysts were successfully prepared via multistep routes in which Ag was uniformly anchored to the enriched Cl sites provided by exfoliated FeOCl nanosheets. Among these Ag–Fe catalysts, 5% Ag–Fe exhibited the highest pseudo first-order kinetic constant 0.1056 min −1 for photo-Fenton degradation of Rhodamine B (RhB), which was 11 times higher than that of FeOCl (0.0096 min −1 ). Ag–Fe catalysts exposed more coordinatively unsaturated Fe active sites to coordinate with H 2 O 2 due to the cleavage of Fe–Cl bond. The exposed coordinatively unsaturated Fe(III) active sites could capture the photoinduced electrons and reduce them to Fe(II), which boosted the separation efficiency of photogenerated charge carriers. Meanwhile, the photogenerated electrons of Ag 0 transferred to the FeOCl, promoting the reduction of Fe(III) to Fe(II). In addition, the intensified visible light adsorption (SPR effect) was achieved after introducing Ag/AgCl nanoparticles on exfoliated FeOCl. Hydroxyl radicals (·OH) and holes (h + ) were determined as the main reactive oxidative species (ROS) in the photo-Fenton degradation process.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2024
·
IF 15.8
Qing Luo,Qian Ma,Taoxia Liu,Yiting Luo,Lianying Wang,Chang Guo,Leyu Wang
We developed an intrinsic hydrophilic single-atom iron nanobowl (Fe-SANB) for magnetic resonance imaging (MRI)-guided tumor microenvironment-triggered cancer therapy. Benefiting from the sufficient exposure of Fe single atoms and the intrinsic hydrophilicity of the bowl-shaped structure, the Fe-SANBs exhibited a superior performance for T1-weighted MRI with an r1 value of 11.48 mM–1 s–1, which is 3-fold higher than that of the commercial Gd-DTPA (r1 = 3.72 mM–1 s–1). After further coembedding Gd single atoms in the nanobowls, the r1 value can be greatly improved to 19.54 mM–1 s–1. In tumor microenvironment (TME), the Fe-SANBs can trigger pH-induced Fenton-like activity to generate highly toxic hydroxyl radicals for high-efficiency chemodynamic therapy (CDT). Both the MRI and CDT efficiency of these nanobowls can be optimized by tuning the ratio of Fe(II)/Fe(III) in the Fe-SANBs via controlling the calcination temperature. Furthermore, the generation of •OH at the tumor site can be accelerated via the photothermal effect of Fe-SANBs, thus promoting CDT efficacy. Both in vitro and in vivo results confirmed that our nanoplatform exhibited high T1-weighted MRI contrast, robust biocompatibility, and satisfactory tumor treatment, providing a potential nanoplatform for MRI-guided TME-triggered precise cancer therapy.
研究领域:
生物医学工程
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纳米医学
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肿瘤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2014
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IF 5.323
Jingu Shi,Zhihui Ai,Lizhi Zhang
In this study we demonstrate Fe@Fe 2 O 3 core–shell nanowires can improve Fenton oxidation efficiency by two times with rhodamine B as a model pollutant at pH > 4. Active species trapping experiments revealed that the rhodamine B oxidation enhancement was attributed to molecular oxygen activation induced by Fe@Fe 2 O 3 core–shell nanowires. The molecular oxygen activation process could generate superoxide radicals to assist iron core for the reduction of ferric ions to accelerate the Fe(III)/Fe(II) cycles, which favored the H 2 O 2 decomposition to produce more hydroxyl radicals for the rhodamine B oxidation. The combination of Fe@Fe 2 O 3 core–shell nanowires and ferrous ions (Fe@Fe 2 O 3 /Fe 2+ ) offered a superior Fenton catalyst to decompose H 2 O 2 for producing OH. We employed benzoic acid as a probe reagent to check the generation of OH and found the OH generation rate of Fe@Fe 2 O 3 /Fe 2+ was 2–4 orders of magnitude larger than those of commonly used iron based Fenton catalysts and 38 times that of Fe 2+ . The reusability and the stability of Fe@Fe 2 O 3 core–shell nanowires were studied. Total organic carbon and ion chromatography analyses revealed the mineralization of rhodamine B and the releasing of nitrate ions. Gas chromatograph-mass spectrometry was used to investigate the degradation intermediates to propose the possible rhodamine B Fenton oxidation pathway in the presence of Fe@Fe 2 O 3 nanowires. This study not only provides a new Fenton oxidation system for pollutant control, but also widen the application of molecular oxygen activation induced by nanoscale zero valent iron .
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2018
·
IF 5.091
Jin Huang,Jie Cao,Ni Tu,Huaping Dong,Jianfa Li,Jianxin Shou,Yimin Li
Nonionic and anionic surfactants often occur in anaerobic environments, but their roles in the removal of organic contaminants by Fe-bearing mineral/Fe(II) have not been determined. In this study, batch experiments were performed to investigate the effects of a nonionic surfactant (TX-100) and an anionic surfactant (SDBS) on the removal of nitrobenzene (NB) by Fe-bearing montmorillonite (FM)/Fe(II). Mössbauer spectrum and XPS were applied to analyze the edge surface bound Fe(II) and secondary minerals formed on FM. The contribution of surfactant to the enrichment of NB on FM was studied. The results showed that TX-100 and SDBS had opposite effects on the removal of NB by FM/Fe(II) at neutral pH. The presence of TX-100 improved the removal efficiency of NB from 36.4% to 70.0%, and increased the initial removal rate by 1.7 times. This enhancement effect was mainly attributed to the formation of more active edge surface bound Fe(II) that can reduce more NB to aniline. Formation of more magnetite on FM and selective enrichment of NB on the reactive surface also contributed to the removal of NB. In contrast, the presence of SDBS reduced the amount of edge surface bound Fe(II) via formation of SDBS-Fe(II) complex, which decreased the removal efficiency of NB.
研究领域:
环境科学
·
矿物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Haiyang Xie,Dan Tang,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Qian He,Hongbing Ji,Tao Gan
The design of non-noble metal single-atom catalysts (SACs) with superior performance for semi-hydrogenation of alkynol to alkenol is remarkable but challenging. Herein, fluorine-tuned Fe SACs supported on N, F-codoped carbon (Fe 1 -NFC) with a Fe-N 4 F 1 structure is successfully prepared via a complexation method. The axial F-doping can modulate the electronic structure of the metalloporphyrin-like active sites (Fe-N 4 ), promoting the transfer of electrons from Fe atoms to F atoms to form electron-deficient Fe δ+ species. As a result, the Fe 1 -NFC catalyst shows a remarkable activity for the semi-hydrogenation of 2-methyl-3-butyn-2-ol to 2-methyl-3-buten-2-ol under mild conditions, with a TOF of 9163 h −1 and a selectivity of 96 % at 97 % conversion, both much higher than that of the Fe SACs supported on N-doped carbon (Fe 1 -NC). Density functional theory (DFT) calculations reveal that the excellent catalytic activity is attributed to the interfacial electronic effect of Fe species induced by axial F-doping, thereby enhancing the exothermic adsorption of alkynol on the Fe-N 4 F 1 structures and accelerating the desorption of alkenol to against the overhydrogenation.
研究领域:
催化
·
材料科学
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化学工程
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Hao Xu,Qian Ye,Jing Zhang,Qiansong Li,Meijing Wang,Peng Zhou,Guanyu Zhou,Qingguo Wang
In response to the inherent restriction of low Fe(II) regeneration in the Fenton process, this study demonstrated a mutual-promoting configuration, where oxygen functionalized g-C 3 N 4 (OCN) was applied in Fe(III)/H 2 O 2 system to utilize mild natural solar light (SL) for persistent Fe(II) generation. The constructed OCN/Fe(III)/H 2 O 2 /SL system exhibited strong adaptability to various pollutants, and it well outperformed the g-C 3 N 4 (GCN) modified system and the traditional Fenton system in pollutants degradation efficiency. Compared with GCN, OCN could significantly promote the Fe(II) generation under solar light (SL), leading to more efficient H 2 O 2 activation. The characterization analyses revealed the larger surface area and enhanced charge separation of OCN, which were considered to take main responsibility for its enhanced photoactivity. The complexation of Fe(III) with the carboxyl groups of OCN also benefited the Fe(II) generation. ·OH was detected as the dominant radical responsible for metronidazole (MNZ) degradation, and its production in the OCN modified system was about twice that in the GCN modified system and the Fenton system. Moreover, the precipitation of FeO x on the OCN surface benefited the charge separation of the OCN, so that the improved OCN enabled a slight enhancement of MNZ degradation in the reuse experiments. The intermediates of MNZ degradation were analyzed based on the results of LC-MS, which provided insight into MNZ degradation pathways. This work highlighted the concept of self-improving photocatalyst, the ingenious combination of photocatalysis and Fenton-like system formed a mutual-promoting situation where the OCN and the Fenton-like system could both be improved, which endowed the configuration great potential for green and economical oxidation in environmental remediation.
研究领域:
环境科学
·
光催化
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水处理
·
高级氧化过程
✓ 已验证
DOI
PubMed
高影响因子
Carbon Energy
·
2025
·
IF 24.2
Zhao Sun,Kun Lei,Louise R. Smith,Nicholas F. Dummer,Richard J. Lewis,Haifeng Qi,Kieran J. Aggett,Stuart H. Taylor,Zhiqiang Sun,Graham J. Hutchings
Advanced oxygen carrier plays a pivotal role in various chemical looping processes, such as CO 2 splitting. However, oxygen carriers have been restricted by deactivation and inferior oxygen transferability at low temperatures. Herein, we design an Fe–O v –Ce–triggered phase-reversible CeO 2− x ·Fe·CaO ↔ CeO 2 ·Ca 2 Fe 2 O 5 oxygen carrier with strong electron-donating ability, which activates CO 2 at low temperatures and promotes oxygen transformation. Results reveal that the maximum CO 2 conversion and CO yield obtained with 50 mol% CeO 2− x ·Fe·CaO are, respectively, 426% and 53.6 times higher than those of Fe·CaO at 700°C. This unique multiphase material also retains exceptional redox durability, with no obvious deactivation after 100 splitting cycles. The addition of Ce promotes the formation of the Fe–O v –Ce structure, which acts as an activator, triggers CO 2 splitting, and lowers the energy barrier of C═O dissociation. The metallic Fe plays a role in consuming O 2− lattice transformed from Fe–O v –Ce, whereas CaO acts as a structure promoter that enables phase-reversible Fe 0 ↔ Fe 3+ looping.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiamin Wei,Qing Wang,Mian He,Shuai Li,Yunan Zhang,Yang Yang,Shipeng Luo,Lianshe Fu,Xin Wang,Tinghai Yang
The development of highly efficient strategy to facilitate comprehensive charge transmission and effective spatial charge separation is expected as a promising approach to improve photocatalytic performance. Herein, the Fe(III) doping modified AgI/NH 2 -MIL-68(In/Fe) Z-scheme heterojunction (ANM-x composite) with unique internal and interfacial charge transmission performance was fabricated by a facile ion exchange precipitation method. The optimized ANM-50 composite exhibits the maximum photocatalytic activity for the degradation of tetracycline, which is about 9.54, 2.61 and 1.86 times higher than that of pure NH 2 -MIL-68In, NH 2 -MIL-68(In/Fe) and AgI, respectively. The characterization results displayed that Ag nanoparticles (NPs) were generated during the photocatalytic procedure, which not only served as a charge transfer-highway, but also reduced the charge flow energy barrier, thereby accelerating charge transfer efficiency and consolidating the stability of the Z-scheme heterojunction. Mechanism exploration reflected that the superior photocatalytic performance was associated with synergetic effect among the introduced Fe(III), constructed ANM Z-scheme heterojunction and the generated Ag NPs, which significantly expands visible light response range and promotes more effective internal and interfacial charge separation. This research not only designs an efficient photocatalyst for decomposing tetracycline, but also opens a new perspective for rational developing Z-scheme heterojunction with unique internal and interfacial charge flow steering.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jinbin Lin,Yuye Hu,Junyang Xiao,Yixin Huang,Mengyun Wang,Haoyu Yang,Jing Zou,Baoling Yuan,Jun Ma
Fe(II)/peracetic acid (Fe(II)/PAA) process exhibits a great potential in abatement of micropollutants because of the fast reaction between Fe(II) and PAA. Similar to Fenton system, the slow reduction from Fe(III) to Fe(II) leads to the high dosage of Fe(II) in Fe(II)/PAA process. This study introduced 2,2′-azino-bis(3-ethylbenz- -othiazoline-6-sulfonate) (ABTS) as electron shuttle to improve the oxidation capacity of Fe(II)/PAA process by accelerating the redox cycle of Fe(III)/Fe(II). ABTS/Fe(II)/PAA process possessed high elimination efficiency of diclofenac in acidic conditions. Alcohols quenching experiments confirmed that ABTS •+ was the primary reactive species responsible for diclofenac elimination, although Fe IV O 2+ and carbon-centered radicals (R-O • ) also existed in ABTS/Fe(II)/PAA process. ABTS •+ was generated via various pathways, including the reactions of ABTS with Fe(III), Fe IV O 2+ and R-O • . ABTS was not an ideal electron shuttle because R-O • could decompose partial ABTS •+ to sulfoxides and sulfones. Two possible degradation pathways of diclofenac were proposed based on the detected transformation products. ABTS/Fe(II)/PAA process was highly-efficient for diclofenac elimination in underground water and reservoir water, while high concentration of humic acid had inhibition effect on diclofenac degradation. The present study provides a promising way to alleviate the intrinsic drawbacks of Fe(II)/PAA process and might advance its potential application in water treatment.
研究领域:
环境科学
·
水处理技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）