WATER RESEARCH
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2025
·
IF 12.4
Rundong Chen,Wenxiao Zheng,Shishu Zhu,Fangshu Qu,Hengyi Fu,Li Tian,Huarong Yu,Jianyi Zhou,Lele Tu,Chunhua Feng
Coagulation with Fe(III) salts is a prevalent phase separation method for organic wastewater treatment. Nevertheless, our industrial applications have shown that using Fe(III) coagulants in landfill leachate treatment leads to an unexpected increase in the bio-toxicity of the effluent. This observation prompts us to identify the toxic compounds and explore their formation mechanisms. Laboratory experiments demonstrate that while Fe(III) coagulation removed approximately 92% of the total organic matter from landfill leachate, it increased the acute bio-toxicity by about 14.5 times relative to the untreated effluent. Molecular analysis of the dissolved organic matter (DOM) in the leachate using Fourier transform ion cyclotron resonance mass spectrometry revealed a significant generation of chlorinated organic compounds during coagulation process. Compared to the Fenton system, the chlorinated compounds formed after coagulation showed a lower oxidation level and predominantly saturated and reduced state. The mechanistic studies suggest that reactive oxygen and chlorine species have a minimal role in the coagulation-induced chlorination. Instead, it is proposed that the redox reaction between Fe(III) and DOM leads to the formation of phenolic radicals, which facilitate nucleophilic reactions with Cl − (as an electron donor), thereby generating chlorinated compounds.
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PubMed
高影响因子
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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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 21
·8952-8959
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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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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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APPLIED CATALYSIS B-ENVIRONMENTAL
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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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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
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胶体与界面化学
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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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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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MOLECULES
·
2023
·Vol. 28
·期 8
·3445
·
IF 4.6
Lei Zhang,Heng Liu,Jiaqi Zhu,Xueling Liu,Likun Li,Yanjun Huang,Benquan Fu,Guozhi Fan,Yi Wang
A novel pyridine-modified chitosan (PYCS) adsorbent was prepared in a multistep procedure including the successive grafting of 2-(chloromethyl) pyridine hydrochloride and crosslinking with glutaraldehyde. Then, the as-prepared materials were used as adsorbents for the removal of metal ions from acidic wastewater. Batch adsorption experiments were carried out to study the impact of various factors such as solution pH value, contact time, temperature, and Fe (III) concentration. The results showed that the absorbent exhibited a high capacity of Fe (III) and the maximum adsorption capacity was up to 66.20 mg/g under optimal experimental conditions (the adsorption time = 12 h, pH = 2.5, and T = 303 K). Adsorption kinetics and isotherm data were accurately described by the pseudo-second-order kinetic model and Sips model, respectively. Thermodynamic studies confirmed that the adsorption was a spontaneous endothermic process. Moreover, the adsorption mechanism was investigated using Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results revealed the pyridine group forms a stable chelate with iron (III) ions. Therefore, this acid-resistant adsorbent exhibited excellent adsorption performance for heavy metal ions from acidic wastewater compared to the conventional adsorbents, helping realize direct decontamination and secondary utilization.Keywords:acidic wastewater;heavy metal ions;pyridine-modified chitosan adsorbent;adsorption mechanism
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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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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Xinna Zhao,Guangbing Liang,Hui Wang,Zhenping Qu
Platinum (Pt) is a nonrenewable mineral with limited reserves and a patchy distribution. Pt demand and consumption are growing year after year. As a result, recovering Pt from the secondary resources is critical. A new strategy for effective Pt recovery employing Fe(III)-oxalate complexes under UV and visible light irradiation is proposed in this paper. This approach can recover 98.9% of Pt in 30 min under the conditions of 365 nm UV irradiation, leaching time = 30 min, C2O42– concentration = 333.33 g/L, and H2O2 addition = 0.60 vol %. More importantly, 95.6% of Pt can also be recovered in 8 h under sunlight. The homogeneous photocatalytic reaction is rapid and efficient, and meanwhile, no strong acid, base, or volatile toxic organic solvent is required. Additionally, the iron utilized in the process may be well-recycled, solving the problem of recovery difficulty of homogeneous photocatalysts and lowering the cost of leaching. Simultaneously, the Pt complex recovered from the waste catalyst is utilized in situ to manufacture 0.1 wt % Pt/ZSM-5 catalyst, which shows the complete conversion of toluene at 200 °C and can remain stable during the long duration reaction of 1200 min. Overall, it can not only provide a new environmentally friendly technique to recycle Pt from spent catalysts but also save manufacturing cost of new catalysts.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 34
·期 2
·2308849
·
IF 19
Yashuai Pang,Minsen Xie,Xinghao Lu,Zhao Wan,Zhuohang Zhong,Waqas Muhammad,Xiang Long Huan,Yinghua Niu,Zhen Zhang,Weiqiang Lv
Lithium–sulfur (Li–S) batteries have attracted wide attention as high-energy-density energy storage devices, but their practical applications are hindered by the severe shuttle effect and sluggish kinetics of lithium polysulfides (LiPSs). To address these challenges, polar mediators are employed to chemisorb and catalyze LiPSs, but most of them suffer from low electronic conductivity and poor catalytic activity. Here, a novel strategy is reported to enhance both properties by dispersing Fe(III) atoms in VO 2 nanoribbons(Fe-VO 2 ), creating electronic metal-support interactions (EMSI) that modulate the electronic structure and charge transfer of VO 2 . Theoretical calculations reveal that EMSI lowers the energy barrier for the decomposition of Li 2 S from 1.60 to 1.32 eV and increases the electronic conductivity of VO 2 . Fe doping reduces the Li-ions diffusion barrier from 1.42 eV in VO 2 to 0.99 eV in Fe-VO 2 . The Fe-VO 2 catalyst shows strong adsorption and fast converstion of LiPSs, resulting in high energy density and long cycling life of Li-S batteries. The cathode with Fe-VO 2 maintains a higher capacity retention of 67% after 500 cycles at 1 C, compared with 52.4% and 53.6% for the carbon black based cathode and VO 2 based cathode, respectively. This work demonstrates the potential of EMSI for designing efficient catalysts for Li–S batteries and provides new insights into the electronic structure engineering of polar mediators.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiahang Liu,Xiaoyang Li,Yingying Chu,Ling Yuan,Ruolin Lv,Weiming Zhang
The conventional Fe(III)/H 2 O 2 system is of low efficiency on the removal of most organic pollutants. However, we discovered that the Fe(III)/H 2 O 2 system was robust on remediating tetracycline (TC) in water (0.109 min −1 for the pseudo-first kinetic constant), and the reaction was even slightly faster than that in the conventional Fe(II)/H 2 O 2 system (0.105 min −1 ). The addition of TC could also initiate the degradation of other refractory pollutants in the Fe(III)/H 2 O 2 system. Complexation between Fe(III) and TC with the stoichiometric ratio of 1:1 was observed. Electron transfer from TC to Fe(III) gave rise to the slight production of Fe(II), which served as the initiator of the following Fenton reaction. •OH was ascertained as the main reactive species through quenching experiments, EPR tests and the probe method, while O 2 • − /HO 2 • was also a subsidiary contributor. Hydroquinone intermediates were proved to be generated through the hydroxylation of the benzene ring of the TC molecule by •OH and thus facilitate the reductive transformation of Fe(III) to Fe(II). This study analyzes the relationship between molecular structural features of TC and the catalytic efficiency of ferric Fenton-like reactions. We expect to shed light on new mechanistic insights on autocatalysis in the Fenton-like catalytic processes.
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