DYES AND PIGMENTS
·
2019
·
IF 4.018
Yingting Zheng,Hailong Wang,Jianzhuang Jiang
A fluorescent porous tetraphenylethylene-based organic polymer ( PTOP ) was constructed by the reaction of 5,5',5'',5‴-(ethene-1,1,2,2-tetrayltetrakis(benzene-4,1-diyl))tetrakis(pyrimidin-2-amine) and cyanuric chloride in the presence of potassium carbonate. CO 2 sorption experiment at 195 K reveals the permanent porosity of PTOP with a Brunauer-Emmett-Teller surface area of 227 m 2 g −1 . In particular, the existence of rich secondary amines and pyrimidine nitrogen atoms surrounding the 1,3,5-triazine moieties in PTOP provides abundant chelating sites for metal ions, endowing a fast-response and sensitive fluorescence sensing Fe(III) with a low limit of detection of 4.5 μM. In addition, this polymer also shows an excellent sensing performance towards nitrobenzene with good selectivity and a low detection limit of 1.6 nM.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 21
·8952-8959
·
IF 3.288
Hehe Qin,Jinhong Fan,Shun Mao
The Fenton method is an important water treatment process. However, the mechanism of the Fenton reaction is still not widely recognized. In this article, the autocatalysis process responsible for the degradation of 4-chlorophenol (4-CP) as well as the generation of Fe(II) and the decomposition of H2O2 is elaborated using a Fe(III)/H2O2 system. It was found that the one electron reduction of Fe(III) to Fe(II) via oxidization of H2O2 to ˙HO2 is not spontaneous according to the standard electrode potential rather than being limited by the rate constant of 0.0027 M−1 s−1 in view of the Haber–Weiss circulation. However, the reaction of Fe(III) and 4-CP is spontaneous with a second-order kinetic rate constant of >0.12 M−1 s−1 and a conversion rate of 0.56%, which triggers the switch of the Fenton-like reaction as a real rate-determining step. The circulation of Fe(III) to Fe(II) in the proposed Fenton-like reaction mechanism depends on the organic species and various intermediates, which indicates its reaction selectivity, preferable for organics with a stronger thermodynamic and kinetic activity. Besides, a slight pH decline with time-scale and the stoichiometric ratio of ˙OH to H2O2 and H2O2 to 4-CP being 1 and 2, respectively, pointed to the new proposed reaction mechanism. The discovery of the new reaction mechanism might promote the theoretical and technical advancement of the Fenton-like process.
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高影响因子
WATER RESEARCH
·
2014
·
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 .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Zhouwei Miao,Xiaogang Gu,Shuguang Lu,Mark L. Brusseau,Xiang Zhang,Xiaori Fu,Muhammad Danish,Zhaofu Qiu,Qian Sui
The performance of Fe(III)-based catalyzed sodium percarbonate (SPC) for stimulating the oxidation of tetrachloroethene (PCE) for groundwater remediation applications was investigated. The chelating agents citric acid monohydrate (CIT), oxalic acid (OA), and glutamic acid (Glu) significantly enhanced the degradation of PCE. Conversely, ethylenediaminetetraacetic acid (EDTA) had a negative impact on PCE degradation, which may due to its strong Fe chelation and HO scavenging abilities. However, excessive SPC or chelating agent will retard PCE degradation. In addition, investigations using free radical probe compounds and radical scavengers revealed that PCE was primarily degraded by HO radical oxidation in both the chelated and non-chelated systems, while O 2 − also participated in the non-chelated system and the OA and Glu modified systems. According to the electron paramagnetic resonance (EPR) studies, the presence of HO in the Fe(III)/SPC system was maintained much longer than that in the Fe(II)/SPC system. The results indicated that the addition of CIT, OA or Glu indeed enhanced the generation of HO in the first 10 min and promoted degradation efficiency by increasing the amount of Fe(III) and maintaining the concentration of HO radicals in solution. In conclusion, chelated Fe(III)-based catalyzed SPC oxidation is a promising method for the remediation of PCE-contaminated groundwater.
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高影响因子
Desalination and Water Treatment
·
2026
·
IF 3.4
Changwei Xiang,Kun Shi,Weiqiang Dong,Huixin Xiong
In this study, ferrihydrite composites of MnO 2 /Fh and PANI/Fh could form from bacterially oxidized Fe(III)-solutions mixing MnCl 2 (Mn/Fe =1) and polyaniline (PANI, 10 mg) at pH 8.0 −10.0, respectively. They could be used to remove P from the (waste)waters. The prepared MnO 2 /Fh wwas identified as Fh, γ-MnO 2 and γ-MnOOH phases by XRD, FTIR and XPS, and the other composite was PANI/Fh. Adsorption processes fitted to the first/second-order rate models and Weber-Morris intraparticle diffusion model (R 2 ranging in 0.920–0.999), and were spontaneous, endothermic and random. Isothermal adsorptions could be well described by Langmuir model (R 2 of 0.991–0.997) and Freundlich model (R 2 of 0.933 −0.979). The maximal P (10 mg/L) adsorption capacities ( Q e ) were 99.3 mg/g (PANI/Fh) and 84.3 mg/g (MnO 2 /Fh), while that of Fh was 53.6 mg/g at pH7.0. There were the wide pH ranges for PANI/Fh (3.0 −11.0) and MnO 2 /Fh (3.0 −8.0), and the presence of CO 3 2- ion declined P removal efficiencies. The main adsorption mechanisms were electrostatic attraction, ion exchange, and surface complexation. Two Fh composites still had the better abilities of treating P-containing neutral river waters after three regenerations. It provides the potential approaches for preparing Fe-composites and removing P using waste bacterial Fe(III)-solutions.
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ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Yanping Bao,Jinhao Lai,Yishun Wang,Zheng Fang,Yongshi Su,Daniel S. Alessi,Nanthi S. Bolan,Xiaolian Wu,Yan Zhang,Xueding Jiang,Zhihong Tu,Hailong Wang
Iron (III) co-precipitation with dissolved organic matter (DOM) is pervasive in many natural environments. However, the effects of DOM on the formation of Fe(III) hydroxysulfate (FHS) and its environmental implications are poorly understood. In this study, fulvic acid (FA) was used as a model DOM compound, and experiments were devised to investigate the effects of FA on the formation of FHS. In addition, the Pb(II) adsorption capabilities of FHSs biosynthesized under various FA dosages, including kinetics and sorption isotherm experiments, were conducted. These experiments showed that co-precipitation of FA promoted the formation of Fe-FA composites, FA-doped schwertmannite , and small particles of jarosite . Co-precipitates are more enriched in carboxyl (–COOH) functional groups due to their preferential binding with FHS. The adsorption kinetics , isotherms and mechanisms of Pb onto the biosynthesized FHSs were then comprehensively characterized and modeled. Though the specific surface area decreased with increasing FA loading, the introduction of FA into FHSs increased Pb(II) adsorption, with the highest concentration of FA addition improving the removal capacity of Pb(II) to 91.54%. Kinetics studies and intra-particle diffusion models indicated that the adsorption of Pb(II) onto the FHSs was correlated with the number of active sites, and two adsorption steps: surface adsorption and the diffusion of Pb(II) in channels inside the biosynthesized FHSs, are suggested. The adsorption mechanism was attributed to cation exchange between Pb(II) and –OH and –COOH functional groups, and the co-precipitated FA provided additional sites for Pb(II) adsorption by FHS.
研究领域:
环境地球化学
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水处理技术
·
胶体与界面化学
·
污染控制化学
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功能材料
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吸附科学
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高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2022
·Vol. 85
·期 7
·2038-2050
·
IF 2.43
Zhang Ming,Zhang Kuo,Zhou Runjuan,Wang Jinpeng
In this study, a new type of iron/copper bimetallic combined with hydroxylamine (HA) activated peroxymonosulfate (PMS) was constructed to treat organic pollutants. Selecting the azo dye acid orange 7 (AO7) as the representative of organic pollutants, the new system can achieve nearly 100% degradation of AO7 within 5 min. The Fe(III)/Cu(II)/HA/PMS system mainly generates SO 4 ·− to achieve the degradation of AO7 in acidic environment, while neutral and alkaline environments rely on · OH. The presence of hydroxylamine accelerates the cycle of Fe(III)/Fe(II) and Cu(II)/Cu(I) in the system, and enhances the degradation ability of the system for organic pollutants. The addition of trace Cu(II) (1 μM) enhances the ability of a single Fe(III)/HA/PMS system to degrade AO7 in neutral and alkaline environments without causing secondary copper pollution. The common inorganic anions Cl − and NO 3 − in water have almost no effect on the degradation of AO7 in the system. The constructed Fe(III)/Cu(II)/HA/PMS system is an efficient and clean organic pollutant wastewater treatment process, which has very promising application prospects. The effect of hydroxylamine on the activation of peroxymonosulfate in Fe(III)-Cu(II) bimetallic is reported for the first time. The Fe(III)/Cu(II)/hydroxylamine/peroxymonosulfate system can remove 100% of AO7 within 5 min. Hydroxylamine enables Fe(III), which cannot activate peroxymonosulfate, to activate peroxymonosulfate efficiently. A trace amount of Cu(II) can reduce Fe(III) to Fe(II).
研究领域:
环境化学
·
高级氧化技术
·
水处理技术
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高影响因子
Journal of Hazardous Materials Advances
·
2026
·
IF 9.1
Wenqi Li,Ying Cao,Quanzhen Yang,He Liu,Stefanos Giannkis,Jin Jiang
UVA-driven iron-mediated sulfite advanced oxidation processes have demonstrated high efficiency in degrading organic pollutants, yet their potential for microbial inactivation remains underexplored. This study systematically investigates the disinfection performance and mechanism of a UVA/Fe(III)/sulfite system using Escherichia coli ( E. coli ) as a model bacterium. The ternary system exhibited synergistic bactericidal activity, achieving complete inactivation of 10 6 CFU/mL E. coli within 45 min at pH 5.6, significantly outperforming individual or binary controls. Radical quenching and electron paramagnetic resonance (EPR) analyses identified sulfate radicals ( SO 4 • − ) , hydroxyl radicals ( • OH ) , superoxide ( O 2 • − ) , and peroxymonosulfate radicals ( SO 5 • − ) as the primary reactive species, generated via a sustained photochemical Fe(II)/Fe(III) redox cycle. Mechanistic investigations revealed a multi-target oxidative cascade: initial disruption of cell envelope integrity and lipid peroxidation facilitated intracellular radical influx, leading to rapid adenosine triphosphate (ATP) depletion, inactivation of antioxidant enzymes (superoxide dismutase (SOD) and catalase (CAT)), and oxidative deoxyribonucleic acid (DNA) lesions. Disinfection efficiency increased with decreasing pH, and was promoted by elevated dissolved oxygen. While chloride and nitrate exhibited moderate interference, phosphate and humic acid severely inhibited inactivation through Fe(III) precipitation and radical scavenging/light screening, respectively. These findings elucidate the inactivation pathways of the UVA/Fe(III)/sulfite system, establishing a theoretical foundation for its application as a cost-effective, solar-driven water disinfection strategy.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Lei Wang,Jianpu Xing,Jianqiao Zhang,Weijun Chen,Mingyan Wang,Yan Li,Yongmin Cao,Wenjie Liu,Weibin Li,Yinghe Zhang,Lei Yang
Highly efficient synergistic catalysis is achieved by constructing a dual two-dimensional MoS 2 /ZnFe-layered double hydroxide composite (2D/2D MoS 2 @ZnFe-LDH) and coupling photocatalysis and Fenton-like process to address the drawbacks of the traditional Fenton-like system. The layered structure of ZnFe-LDH enables firm anchoring and uniform dispersion of Fe active sites within the layers without forming clusters, meanwhile enhancing mass transfer efficiency and accelerating both peroxymonosulfate (PMS) adsorption and reactive oxygen species desorption. The constructed 2D/2D heterojunction strengthens interfacial covalent bonding and compatibility, shortens the migration distance of photogenerated carriers, thereby significantly improving the charge separation efficiency, which accelerates the Fe(III)/Fe(II) cycle for sustainable catalysis across a broad pH range without Fe sludge aggregation. Comprehensive analysis of EPR, in-situ XPS, quenching and probe experiments, and DFT indicates that PMS is efficiently adsorbed onto Fe sites and reduced to generate SO 4 •- and •OH. Meanwhile, further characterization combining EPR, determination of surface Fe(II) concentration, in-situ photoelectrochemical and Raman measurements, XPS and DFT confirms that photogenerated electron can simultaneously reduce Fe(III) and promote radical desorption, thereby achieving sustainable catalysis. Hence, the system achieves complete phenol removal with a high synergistic index and figure of merit of 9.69 and 2.62 × 10 −10 mol·L −1 ·h −1 ·g −1 ·J −1 , respectively. It also operates efficiently in various complex water matrices and maintains stable operation over 24 h in the continuous-flow reactor, demonstrating strong anti-interference capability without any biological toxicity. In conclusion, this study proposes a new strategy to develop for developing high-performance and sustainable photo-Fenton-like dual-system.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Yang Liu,Fenxian Cun,Dongqi Tian,Peng Zhou,Yue Yuan,Zhaokun Xiong,Chuanshu He,Ye Du,Zhicheng Pan,Bo Lai
Sodium bismuthate dihydrate (NaBiO 3 .2 H 2 O, NBH) nanosheets were successfully prepared in this study using the persulfate oil bath oxidation method. Benefited from the unique layered structure of NBH, the Fe(III) as a variable valence metal ion was explored for enhancing NBH activation of peroxymonosulfate (PMS) to degrade levofloxacin (LVF) in the visible-light catalytic system. Based on results of the reactive oxygen species (ROS) quenching experiments and electron paramagnetic resonance (EPR) analysis, singlet oxygen ( 1 O 2 ) and superoxide radical (O 2 ·- ) were identified as the main ROS. The morphology, chemical structure, and optical properties of NBH were analyzed using various characterization methods. It was confirmed that Fe(III) embedded in the NBH via the ion exchange with Na, resulting in lattice oxygen vacancies on the surface of the NBH, after the formation of oxygen defect sites, reacts with PMS in the solution to produce active oxygen species with oxidizing efficiency. This study expands the technological application of NBH in the catalytic oxidation of variable valence metals, which are essential for the removal of fluoroquinolone antibiotics.
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DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Xiang Liang,Wenhui Feng,Dong Liang,Yan Xu,Xiaoqing Qiu
Hydroxyl/amino and Fe(III) co-grafted graphite carbon nitride (CN) is fabricated via alkaline hydrothermal treatment and followed by an impregnation adsorption process. In this unique fabrication, hydroxyl and amino groups enriched on the surface play a vital role in improving the adsorption capacity for volatile organic compounds (VOCs), while the grafted amorphous Fe(III) clusters could dominantly regulate the path of molecular oxygen activation via photo-Fenton reaction, and change the selectivity of intermediate reactive oxygen species (ROS) with the assistant of the rich surficial hydroxyl groups. Meanwhile, both the grafted functional groups and Fe(III) clusters can serve as photogenerated charge acceptors for collaboratively accelerating carriers' separation. Besides, the Fe(III)-mediated interfacial charge transfer effect (IFCT) also could extend visible light absorption and boost carriers’ generation. Benefiting from the virtues of the complementary and synergy of the grafted hydroxyl/amino and Fe(III), the dual-functionalized CN is qualified as an efficient photocatalyst for removal of VOCs, which exhibits 22 and 18 times isopropanol (IPA) adsorption capacity and CO 2 production than of pristine CN during photocatalytic IPA removal, respectively. Moreover, this work provides a new strategy of surficial group-cluster bifunctionalization for systematically improving sustainable solar-to-chemical energy conversion towards VOCs mineralization.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Tao Pan,Yu Wang,Xin Yang,Xiong-fei Huang,Rong-liang Qiu
Fe(II)-catalyzed peroxymonosulfate (PMS) activation process was able to degrade persistent organic pollutants, such as polybrominated diphenyl ethers (PBDEs), but the slow transformation rate from the generated Fe(III) to Fe(II) restricted the efficiency of this process. In this study, we found that the addition of small quantities of gallic acid (GA), a model compound of natural polyphenols, in the Fe(III)/PMS process (namely GA/Fe(III)/PMS process) could exert a long-term influence on Fe(II) recycle and accelerated the degradation of 2,2′,4,4′-tetrabromodiphenyl ether (BDE47) over 72 h. Under conditions of 20.3 µM GA, 13.6 µM Fe(III) and 400 µM PMS, the degradation efficiency of BDE47 reached 85%, which was 9.4 times higher than that in the Fe(III)/PMS process. The degradation kinetics can be divided into an initial “fast stage” (k obs1 = 0.298 h −1 ) and a second “slow stage” (k obs2 = 0.021 h −1 ). Aromatic radicals such as hydroxycyclohexadienyl radical (poly-HCD ) produced by the attack of SO 4 − /HO on GA was proposed to be responsible for Fe(II) recycle in the first stage, while ring-opened products following SO 4 − /HO attack of GA-quinone mainly initiated Fe(III) reduction in the second stage. Owing to the multiple Fe(III) reduction pathways, PMS would be continuously activated by Fe(II) to form SO 4 − and HO , which were the dominant reactive species for BDE47 degradation. Finally, natural polyphenols extracted from green tea were proven effective in enhancing BDE47 degradation in Fe(III)/PMS process. This study not only provides a new way to propagate Fe(II)-activated persulfate chain reactions for the degradation of refractory organic contaminants, like PBDEs, but also sheds new insight into the reactivity of organic byproducts toward Fe in PMS-based oxidation system.
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高影响因子
危险品化学品经营许可证（带存储）