NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 22
·10857-10865
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IF 3.3
Jinglin Zhu,Meng Zhu,Juanjuan Peng
Developing highly active Fenton-like materials for the decontamination of water is a hot topic. Nanosized Fe3O4 particles are green catalysts for environmental remediation, but their application is limited by their low catalytic activity. Herein, Fe3O4 rhombic dodecahedral nanoparticles (Fe3O4-R) with exposed {110} facets were synthesized via the solvothermal method and used as a Fenton-like catalyst for the degradation of bisphenol A (BPA). Consequently, ∼100% of BPA was removed using Fe3O4-R/H2O2 at pH = 5.0, which was higher than that by commercial Fe3O4. Multiple experiments confirmed the presence of abundant Fe(II) active sites on the surface of Fe3O4-R, but they were unstable, resulting in the dissolution of Fe(II) from the solid surface via oxidation, and thus the homogeneous reaction was not negligible in the Fe3O4-R/H2O2 process. However, hydroxyl radicals (HO˙) were still the primary reactive species, playing a dominant role in the removal of BPA. Consequently, the degradation of BPA was easily disturbed by HCO3− and natural organic matter (NOM). Unfortunately, the inactivation of Fe3O4-R was observed in cycle experiments, which is ascribed to the stabilization of the surface of Fe3O4-R during the oxidation process, reducing the surface active sites of Fe(II). Therefore, this study provides new insight into the Fenton-like oxidation process for the degradation of pollutants by regulating the morphology of Fe3O4 nanoparticles.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
·
IF 6.9
Xueqian Wu,Zhen Li,Jiangyan Tao,Yufei Xie,Wei Liu,Songjian Zhao
The Fenton technology used for treating formaldehyde-containing wastewater (HCHO) has limitations in terms of pH, efficiency, and cost. To address these issues, a Fe x -HT Fenton-like catalyst was developed in this study. This catalyst combines active Fe with walnut shell biochar (HT) that contains surface defects, resulting in a highly effective solution for the rapid purification of formaldehyde wastewater in complex environments. The carbon defects on the HT surface play a crucial role in stabilizing the active Fe binding, while the appropriate loading of Fe further enhances the specific surface area of HT. Additionally, the porous structure of HT provides ample contact sites for formaldehyde. Furthermore, the Fe 3 -HT catalyst exhibits superparamagnetism, allowing for convenient recovery of the catalyst after use. Experimental results demonstrate that Fe 3 -HT achieves an impressive 90% degradation rate for systems containing HCHO concentrations ranging from 200 to 800 mg/L. The effects of feed ratio, pH, and formaldehyde concentration on the performance of Fe 3 -HT were thoroughly investigated. Moreover, a possible mechanism for the degradation of HCHO by the Fe 3 -HT Fenton-like catalyst was proposed. The environmentally friendly catalyst developed in this study boasts numerous advantages, including low cost, high treatment capacity for wastewater, and strong adaptability to complex wastewater environments.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Jinglin Yin,Junhui Yang,Yanmei Li,Ziyang Xiang,Ting Yang,Jing Wang,Tao Xu,Qiong Wang,Wenlei Wang
This study investigated the Fenton-like oxidation of As(III) by three types of iron oxides in oxalate systems. The effects of pH, oxalate concentration and atmosphere on the oxidation of As(III) by iron oxide photocatalyst were studied. Firstly, hydrothermal carbon (HTC) was used as the carrier to load three kinds of iron oxides to prepare new composite materials, including α–FeOOH, α Fe 2 O 3 and Fe 3 O 4 , which can solve the dispersion problem of iron oxide by using a large number of rich functional groups on the HTC surface. The experiment results showed that under the conditions of O 2 , pH = 5.0 and oxalate concentration of 0.5 mmol·L 1 , As(III) was completely oxidized by α–FeOOH and α–Fe 2 O 3 at 15 min and 20 min, respectively. Density functional theory (DFT) was used to study the surface adsorption energy of iron oxide and oxalate. The calculated results showed that the order of adsorption energy of three iron oxides for the oxalate is α FeOOH > α Fe 2 O 3 > Fe 3 O 4 . Fe III (C 2 O 4 ) + , a mononuclear bidentate iron oxalate chelate with the strongest photosensitivity , was constructed in the Fe-Oxalate system containing only Fe(III), resulting in the photocatalytic efficiency of α–FeOOH and α Fe 2 O 3 was superior to that of Fe 3 O 4 . These findings contribute to arsenic remediation of water bodies by using iron materials and oxalate in the natural environment.
研究领域:
环境科学
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化学
✓ 已验证
DOI
高影响因子
Scientific Reports
·
2016
·Vol. 6
·期 1
·1-11
·
IF 5.228
Xiang Wei,Zhang Beiping,Zhou Tao,Wu Xiaohui,Mao Juan
This study demonstrated the synergistic degradation of 4-chlorophenol (4-CP) achieved in a magnetic field (MF) enhanced zero-valent iron (ZVI)/H 2 O 2 Fenton-like (FL) system and revealed an interesting correlative dependence relationship between MF and the pristine iron oxides layer (Fe x O y ) on ZVI particles. First, a comparative investigation between the FL and MF-FL systems was conducted under different experimental conditions. The MF-FL system could suppress the duration of initial lag degradation phase one order of magnitude in addition of the significant enhancement in overall 4-CP degradation. Monitoring of intermediates/products indicated that MF would just accelerate the Fenton reactions to produce hydroxyl radical more rapidly. Evolutions of simultaneously released dissolved iron species suggested that MF would not only improve mass-transfer of the initial heterogeneous reactions, but also modify the pristine ZVI surface. Characterizations of the specific prepared ZVI samples evidenced that MF would induce a special evolution mechanism of the ZVI particles surface depending on the existence of Fe x O y layer. It comprised of an initial rapid point dissolution of Fe x O y and a following pitting corrosion of the exposed Fe 0 reactive sites, finally leading to appearance of a particular rugged surface topography with numerous adjacent Fe 0 pits and Fe x O y tubercles.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Sijing Yao,Jianqing Ma,Di Ma,Mika Erik Tapio Sillanpää,Minghua Zhou,Qing Ye,Huixia Jin,Kefeng Zhang
Chromium, as a widely utilized transition metal, presents wastewater with high toxicity and challenging treatment. To date, there has been limited exploration regarding the application of chromium in homogeneous Fenton-like reactions. This study aims to explore the potential of Cr(VI) and Cr(III) to activate hydrogen peroxide (H 2 O 2 ) and permonosulfate (PMS) for degrading coexisting pollutants in homogeneous solutions. The Cr(VI)/PMS system was found to be the most effective, with a 95.58 % removal efficiency for the azo dye Acid Red 73 (AR73). The Cr(VI)/H 2 O 2 system followed with 72.35 %, while the Cr(III)/H 2 O 2 and Cr(III)/PMS systems showed lower efficiencies at 25.65 % and 16.95 %, respectively. Various techniques were employed to delve into the mechanisms underlying chromium activation. The results indicate that both Cr(VI) and Cr(III) can activate H 2 O 2 to generate hydroxyl radical (HO • ). Moreover, Cr(VI) can activate PMS in the pH range of 3 ∼ 11, producing HO • , sulfate radical (SO 4 •- ), and singlet oxygen ( 1 O 2 ), while Cr(III) engages in chelation with PMS, causing the reaction to cease. Additionally, this study reveals that the chelating agent EDTA, upon complexing with Cr(III), efficiently activates PMS to generate 1 O 2 , and the mechanism behind EDTA-Cr(III) activation of PMS was elucidated through DFT calculations. An integrated evaluation of Cr performance in the Fenton-like reaction provides new research directions for the removal of pollutants from chromium-containing wastewater.
研究领域:
环境科学
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化学工程
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污染控制
✓ 已验证
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DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2017
·
IF 2.084
Ruixia Shi,Yan Zhang,Xingtao Wang,Qian Ma,Aiyu Zhang,Ping Yang
Porous ZnFe 2 O 4 nanotubes and nanobelts have been fabricated through an efficient and facile approach of electrospinning followed by two-step calcination in atmosphere. The influences of electrospinning parameters such as metallic salt content, PVP content, the ratio of ethanol to water, stirring time and applied voltage on the composite fibers have been fully investigated. When the calcination temperature was increased from 600 °C to 650 °C, the ZnFe 2 O 4 nanotubes evolved into well-crystalline nanobelts due to the faster gas diffusion , more active grain growth and atomic diffusion rate caused by the relative high temperature. The plausible formation mechanism of ZnFe 2 O 4 nanotubes and nanobelts was proposed and discussed in detail. The photocatalytic activities for the photo-degradation of Rhodamine B (RhB) over ZnFe 2 O 4 nanotubes and nanobelts were evaluated under the UV-light irradiation. The degradation efficiency of nanotubes and nanobelts both can reach 99.7% after 20 min UV irradiation in presence of H 2 O 2 because of synergistic effects of Fe 3+ and H 2 O 2 , respectively, indicating the excellent Fenton-like photocatalytic properties of ZnFe 2 O 4 nanotubes and nanobelts. Additionally, the Fenton-like photocatalytic mechanism was also discussed.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
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IF 7.864
Chao Shan,Hui Liu,Ming Hua,Bingcai Pan
The development of catalysts for oxidation of aqueous contaminants has long been relying on trial-and-error strategies due to lack of activity-tuning principles. Herein, Fenton-like oxidation of As(III) as a chemisorbed model contaminant over a series of fabricated CexTi1-xO2 catalysts with tunable structures was investigated. The activity of CexTi1–xO2 showed a volcano-shape dependency on Ce molar fraction, peaking at Ce0.25Ti0.75O2 (x = 0.25) with 6.32–6.36 times higher activity and 2.67–2.94 times higher specific activity compared with CeO2 and TiO2. The non-radical surface hydroperoxo complexes were experimentally substantiated as the dominant oxidant species on Ce0.25Ti0.75O2, which enabled a high efficiency of H2O2 utilization (99.1%). Under the verified Langmuir–Hinshelwood mechanism, the microkinetic model for the catalytic oxidation was established, and thus, the quantitative relationship between activity and adsorption energies for bimolecular chemisorption reactions was elucidated. Theoretically, a catalyst with identical adsorption energies toward both chemisorbed reactants tends to obtain the highest activity. Through DFT calculation, the highest activity of Ce0.25Ti0.75O2 was rationally interpreted by the balanced adsorption energies toward As(III) and H2O2, which was attributed to the shifted electronic density of states induced by Ce doping. This study provides a potent strategy to tune the catalytic activity of bimolecular chemisorption reactions.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 8
·7810-7820
·
IF 2.914
Zou Haiyuan,Ning Xun-an,Wang Yi,Sun Jian,Hong Yanxiang
In this paper, a novel strategy integrating ultrasound (US) with a Fenton-like (zero-valent iron/EDTA/air, ZEA) process was proposed for the removal of the refractory and carcinogenic aromatic amines (AAs) in textile dyeing sludge for the first time. The operating condition was optimized as 1.08 W/cm 3 ultrasonic density, 15 g/L ZVI, and 1.0 mM EDTA, which could reach degradation efficiencies of 51.79% in US, 72.88% in ZEA, and 92.40% in US/ZEA system after 90-min reaction. Quenching experiments showed that electron transfer reactions generated by the iron ligands in ZEA brought about various reactive oxidative species (ROS), in which Fe (IV), O 2 ˙ − , and ˙OH dominated the degradation. US induced sludge disintegration by ultrasonic shear, proven by particle size decrease and supernatant organic matter upsurge, which helps ROS contact with those pollutants in the sludge cavities. Besides, US facilitated the iron redox cycle for oxygen activation by promoting the corrosion of ZVI and stripping considerable ferric ions from sludge iron oxides which were verified by SEM, XRF, and XPS.
Graphical abstract
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
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2023
·
IF 8.9
Fei Wang,Mingming Zhang,Xingyu Liu,Zimeng Li,Hongkai Zhu,Fei Lian,Xiangyue Liu,Liqiang Li,Xintian Wu,Hongwen Sun
The traditional Fenton system is subject to the low efficiency of the Fe(III)/Fe(II) conversion cycle, with significant attempts made to improve the oxidation efficiency by overcoming this hurdle. In support of this goal, iron-enriched sludge-derived hydrochar was prepared as a high-efficiency catalyst by one-step hydrothermal carbonization and its performance and mechanisms in mediating the oxidation of triclosan were explored in the present study. The hydrochar prepared at 240 °C for 4 h (HC 240-4 ) had the highest removal of triclosan (97.0%). The removal of triclosan in the HC 240-4 /H 2 O 2 system was greater than 90% in both acidic and near-neutral environments and remained as high as 83.5% after three cycles, indicating the broad pH applicability and great recycling stability of sludge-derived hydrochar in Fenton-like systems. H 2 O 2 was activated by both persistent free radicals (PFRs; 19.7%) and iron (80.3%). The binding of Fe(III) to carboxyl decreased the electron transfer energy from H 2 O 2 to Fe(III), making its degradation efficiency 2.6 times greater than that of the conventional Fenton reaction . The study provides a way for iron-enriched sludge utilization and reveals a role for hydrochar in promoting iron cycling and electron transfer in the Fenton reaction.
研究领域:
环境科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Dingxi Zhang,Yuping Xiang,Guangliang Liu,Lina Liang,Lufeng Chen,Jianbo Shi,Yongguang Yin,Yong Cai,Guibin Jiang
Methylmercury (MeHg), derived from industrial processes and microbial methylation , is still a worldwide environmental concern. A rapid and efficient strategy is necessary for MeHg degradation in waste and environmental waters. Here, we provide a new method with ligand-enhanced Fenton-like reaction to rapidly degrade MeHg under neutral pH. Three common chelating ligands were selected (nitriloacetic acid (NTA), citrate, and ethylenediaminetetraacetic disodium (EDTA)) to promote the Fenton-like reaction and degradation of MeHg. Results showed that MeHg can be rapidly degraded, with the following efficiency sequence: EDTA > NTA > citrate. Scavenger addition demonstrated that hydroxyl radical ( ▪ OH), superoxide radical (O 2 ▪– ), and ferryl (Fe Ⅳ O 2+ ) were involved in MeHg degradation, and their relative contributions highly depended on ligand type. Degradation product and total Hg analysis suggested that Hg(Ⅱ) and Hg 0 were generated with the demethylation of MeHg. Further, environmental factors, including initial pH, organic complexation (natural organic matter and cysteine), and inorganic ions (chloride and bicarbonate) on MeHg degradation, were investigated in NTA-enhanced system. Finally, rapid MeHg degradation was validated for MeHg-spiked waste and environmental waters. This study provided a simple and efficient strategy for MeHg remediation in contaminated waters , which is also helpful for understanding its degradation in the natural environment.
研究领域:
环境科学
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2019
·
IF 2.584
Ting Chen,Zhiliang Zhu,Hua Zhang,Xiaolin Shen,Yanling Qiu,Daqiang Yin
The study on the removal of refractory veterinary antibiotic florfenicol (FF) in water is still very limited. In this study, an efficient Fenton-like catalyst was developed by synthesizing a series of Cu-based multi-metal layered double hydroxides (CuNiFeLa-LDHs) to degrade FF in aqueous solution. In the experiments, the screened CuNiFeLa-2-LDH with the molar ratio of La3+/(Fe3+ + La3+) = 0.1 exhibited high catalytic activity, achieving almost complete degradation of 5 mg L–1 FF under 5 mmol L–1 H2O2 conditions. The mechanisms revealed that the enhanced catalytic performance was ascribed to the existence of Ni which accelerated the electron transfer rate and La which served as a Lewis acidic site to provide more reactive sites in this Cu-dominated Fenton-like reaction, further generating •OH, •O2–, and O21 as active species to attack pollutants directly. Interestingly, the catalyst showed a wide pH adaptability and little release of copper ions to the solution. The regenerated CuNiFeLa-2-LDH is demonstrated to be a stable and reliable material for florfenicol degradation.
研究领域:
环境科学
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催化化学
·
兽医学
✓ 已验证
DOI
PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2024
·
IF 4.3
Jing Yang,Yu Du,Wenpeng Li,Shaoyun Shan,Tianding Hu,Hongying Su
Adsorption has been applied as a useable technique for the treatment of tetracycline (TC) contaminated wastewater, however, complete removal of TC without secondary contamination using adsorption is still challenging. Recently, new strategies by coupling adsorption with degradation protocol are considered as promising candidate for water treatment. Herein, iron oxide nanoparticle-doped hydrogel particles (Fe 3 O 4 @SiO 2 –NH 2 /SA) were prepared by introducing amino-functionalized Fe 3 O 4 @SiO 2 into Fe 2+ -crosslinked alginate hydrogel and evaluated as adsorbent-promoted catalyst for TC removal via adsorption-coupled Fenton-like reaction (ACFLR). These composite particles can effectively adsorb TC molecules by π-π interaction, hydrogen bonding and electrostatic interaction, leading to a relatively high adsorption capacity at 588.41 mg g −1 . Interestingly, the adsorption and concentration of TC on the adsorbent would facilitates its degradation via Fenton-like reaction, since the decreased distance of neighboring TC and Fenton-like catalytic sites enhanced the efficiency of short-lived reactive oxygen species. The removal efficiency of TC by ACFLR was up to 98.76% at 4 h, which is strongly enhanced compare to that obtained by adsorption alone (44.73%). Results above indicate that the hydrogel composite is potential adsorbent-promoted catalyst for the effective removal of TC in aqueous environment via ACFLR.
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
危险品化学品经营许可证（带存储）