INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Weisheng Dai,Yao Wang,Weijuan Guo,Guofu Wang,Muqing Qiu
The effects of Fe(II) and humic acid on U(VI) immobilization onto oxidized carbon nanofibers (Ox-CNFs, pyrolysis of bacterial cellulose) were investigated by batch, spectroscopic and modeling techniques, with results suggesting that, Ox-CNFs exhibited fast adsorption rate (adsorption equilibrium within 3 h), high adsorption performance (maximum adsorption capacity of 208.4 mg/g), good recyclability (no notable change after five regenerations) in the presence of Fe(II) towards U(VI) from aqueous solutions (e.g., 40 % reduction and 10 % adsorption at pH 8.0), which was attributed to the various oxygen-containing functional groups, excellent chemical stability, large specific surface area and high redox effect. U(VI) adsorption increased with increasing pH from 2.0 to 5.0, then high-level plateau and remarkable decrease were observed at 5.0–6.0 and at pH > 6.0, respectively. According to FT-IR and XPS analysis, a negative correlation between U(VI) reduction and organic in the presence of Fe(II) implied that U(VI) reduction was driven by Fe(II) while inhibited by humic acid. The interaction mechanism of U(VI) on Ox-CNFs was demonstrated to be adsorption and ion exchange at low pH and reduction at high pH according to XPS and surface complexation modeling. These findings filled the knowledge gaps pertaining to the effect of Fe(II) on the transformation and fate of U(VI) in the actual environment. This carbon material with distinctive performance and unique topology offers a potential platform for actual application in environmental remediation.
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高影响因子
Frontiers in Chemistry
·
2025
·
IF 4.2
Xianbing Zhang,Yuheng Liu,Jiajia Yuan
Metal-organic frameworks (MOFs) are recognized as important Fenton-like materials for environmental remediation. However, their applications are often hindered by slow cycling between Fe (III) and Fe (II). This study aimed to address the slow Fe (III)/Fe (II) cycling limitation of Fe-MOFs through dual modification strategy: bimetallic modification and amino functionalization. A series of NH2-MOF(Fe, Co) catalysts with varying Fe/Co ratios were synthesized via a hydrothermal method and evaluated for sulfamethoxazole (SMX) degradation. The optimized NH2-MOF(Fe, Co) catalyst (Fe/Co ratio = 7:3) exhibited substantially enhanced catalytic performance, with SMX removal rate and rate constant in the H2O2 system being 3.2 and 43.5 times higher than those of the Fe-MOF/H2O2 system, respectively. The catalyst demonstrated robust performance across a wide pH range (3.05–7.00), addressing a common limitation of Fenton-like systems. Physicochemical characterization revealed that the enhanced performance was attributed to two key factors: the synergistic effect between Co and Fe in the bimetallic active center, and improved electron transfer to the central metal due to -NH2 functionalization. These modifications effectively addressed the Fe (III)/Fe (II) redox cycling limitation. The proposed reaction mechanism provides insights into SMX degradation pathways in the NH2-MOF(Fe, Co)/H2O2 system. This study presents an efficient and stable MOF-based Fenton-like catalyst with potential applications in wastewater treatment and environmental remediation.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2025
·Vol. 39
·期 5
·e70103
·
IF 0
Palanisamy Vasudhevan,Dong Yu,Ruoyu Zhang,Mysoon M. Al-Ansari,Velu Manikandan,Hui Ma,Saurav Dixit,Shengyan Pu
Chlorinated aromatic chemicals are highly hazardous, transmissible, and bioaccumulative. Developing an economically feasible catalytic method to facilitate the effective removal of chlorinated aromatic pollutants is critical for contamination prevention. The current study extensively investigated the utilization of organic ligands such as citrate (CA) and ethylenediaminetetraacetic acid (EDTA) to increase Fe(II)-activated persulfate (PS) for 4-chlorophenol (4-CP) and 3-chlorobenzoic acid (3-CB) degradation in water. The decomposition and consumption ability of persulfate in PS alone and Fe(II)/PS systems for 4-CP and 3-CB was very low because of the rapid utilization as well as discontinuous availability of Fe(II), which indicates the decline of Fe(III) to Fe(II). But, when using the citrate/Fe(II)/PS and EDTA/Fe(II)/PS combinations, the degradation of 4-CP and 3-CB was 78.86%, 75.01% and 84.84%, 80.99% within 30 min, respectively. The significant enhancement is due to both ligand-to-metal transfer of charges process, and this increased the process of rate determination through carrying electrons into the citrate and EDTA ligands to Fe(III), generating Fe(II). In addition, the 4-CP and 3-CB degradation facilitated with citrate/Fe(II)/PS and EDTA/Fe(II)/PS systems was efficiently degraded at acidic pH (2.0–6.0) conditions. The pseudo-first-order kinetics model accurately predicted 4-CP and 3-CB degradation in the organic ligand/Fe(II)/PS systems. The degradation percentage of 4-CP and 3-CB increased with increasing PS and Fe(II) concentrations. Moreover, both sulfate and hydroxyl radicals formed by citrate/Fe(II)/PS and EDTA/Fe(II)/PS systems were identified as major reactive oxygen species for 4-CP and 3-CB decomposition. The present investigation recommends an alternate strategy to enhance the Fe(II)-activated persulfate mechanisms.
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WATER RESEARCH
·
2020
·
IF 9.13
Panpan Wang,Xiaolin Liu,Wei Qiu,Feihong Wang,Haicheng Jiang,Mansheng Chen,Wei Zhang,Jun Ma
Low cost, green, regenerable catalyst for persulfate activation is the popularly concerned topic for the degradation of persistent organic micropollutants in drinking water . In this work, natural montmorillonite (MMT) saturated with Fe(III) ions was used to activate peroxymonosulfate (PMS) for the degradation of atrazine in raw drinking water. Results showed that the adsorption of atrazine was quickly completed within 1 min and the percentage degradation was finally increased up to 94.1% in 60 min. The d 001 -spacing of MMT was enlarged to 2.91 nm at the most by Fe(III) saturation. Atrazine was adsorbed into the nanoscale interlayer of Fe(III)-saturated montmorillonite (Fe-MMT), where the Fe(III)/Fe(II) cycle was sustainably realized through the accelerated transformation of electrons between Fe(III) and PMS. Meanwhile, the in-situ generated Fe(II) accelerated the decomposition of PMS to further proceed the degradation of atrazine through the oxidation of HO• and SO 4 • - radicals. This nanoconfined effect of PMS activation by Fe(III) was further confirmed through the degradation of various micropollutants in the backgrounds of river water. The selective catalytic oxidation of micropollutants through PMS activation was attributed to the 2D mesoporous structure of Fe-MMT, inhibiting the interlayer adsorption of larger molecular backgrounds (humic acids etc. ). Fe(III)-saturated montmorillonite (Fe-MMT) provided a feasible and scalable method of PMS activation by Fe(III) for the degradation of micropollutants in drinking water.
研究领域:
环境科学
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催化材料
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FOOD HYDROCOLLOIDS
·
2026
·
IF 13.8
Ying Li,Xiaoyu Yang,Liang Li
To address the technical challenge of balancing the stability and bioavailability of conventional iron supplements, this study developed a plant-based composite gel system in which Fe(II) served as both a nutritional factor and an ionic crosslinker. The results showed that the three-dimensional gel network was primarily maintained by hydrophobic interactions. Two-dimensional correlation analysis further indicated that Fe(II) may coordinate with the carboxyl groups of sodium alginate (SA) to form ionic bridges, triggering the dissociation and reconstruction of the hydrogen-bonding network, subsequently inducing soy protein isolate (SPI) conformational unfolding, thereby regulating gel network formation. At an Fe(II) concentration of 0.25%, the in-situ ionic crosslinking degree reached the optimum level, yielding a gel with a hardness of 55.72 ± 0.27 g, the highest storage modulus, and the most uniform pore distribution. The β-sheet content in the SPI secondary structure reached its maximum (38.40%), effectively retarding Fe(II) diffusion and gastrointestinal loss. Overall, this study elucidated the mechanism of Fe(II)-mediated in-situ ionic crosslinking and established the structure–function relationship among crosslinking degree, gel structure and Fe(II) controlled-release behavior. These findings provide a novel food-grade iron supplement for alleviating iron-deficiency anemia and expanding the application of plant protein-based composite gels in active mineral delivery.
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RSC Advances
·
2026
·Vol. 16
·期 18
·16505-16511
·
IF 6.1
Cong Gao,Houfen Li,Jize Liu,Wenchao Yang,Hong Chen,Jianbo Han
The heterogeneous Fenton-like reaction is a promissing technology for removing organic pollutants in water. The reduction of Fe(III) to Fe(II), as the rate-limiting step for generating ˙OH, is crucial in heterogeneous Fenton-like reactions and may be improved using organic pollutants with lower redox potential than that of Fe(III)/Fe(II). In this work, the rapid reduction of Fe(III) to Fe(II) on the MIL-100-Fe catalyst was achieved by degrading methylene blue (MB, E0 = 0.01 V), which has the desired lower redox potential than that of MIL-100-Fe(III)/Fe(II) (E0 = 0.76 V). By contrast, organic pollutants with higher redox potentials than that of MIL-100-Fe, such as phenol (E0 = 0.97 V) and p-nitrophenol (E0 = 1.23 V), were incapable of reducing Fe(III) to Fe(II). As a result, the degradation rate constant of MB was one order of magnitude higher than those of phenol and p-nitrophenol. Notably, MB could also promote the reduction of Fe(III) to Fe(II) in the presence of phenol or p-nitrophenol; thus, the degradation rate constants of phenol and p-nitrophenol were significantly enhanced by 50 and 30 times, respectively. The results revealed that organic pollutants with lower redox potential than that of Fe(III)/Fe(II) could facilitate the reduction of Fe(III) to Fe(II), which is beneficial for producing more ˙OH, thus improving the heterogeneous Fenton-like catalytic performance.
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JOURNAL OF THE INDIAN CHEMICAL SOCIETY
·
2026
·Vol. 103
·期 5
·102557
·
IF 3.4
Lei Liu,Fang Liu,Xinqian Ma,Jingyue Qian,Qiangshun Wu,Lina Wang,Liqiang Cui
Iron-based metal organic frameworks (Fe-MOFs) have been regarded as the ideal precursors for synthesis of iron-carbon micro-electrolysis (IC-ME) materials. However, their conventional autoclave-based fabrication limits large-scale application, and the potential of the resulting Fe@C composites derived from Fe-MOFs for Cr(VI) reduction remains underexplored. Herein, a facile stirring method conducted under ambient conditions was successfully developed. The evolution from Fe-MOFs to Fe@C was comprehensively characterized, and its reductive capacity for Cr(VI) was systematically evaluated. The effect of key experimental parameters including reaction time, initial pH value, electrolyte concentration, catalyst dosage, and environmental matrices on Cr(Ⅵ) removal were investigated in detail on the basis of the concentration variation of Fe ions released into water. The obtained results indicated that the rate of Cr(VI) removal-efficiency change (Δη/Δt) was positively corelated with that of Fe(II) concentration change (Δ C Fe(II) /Δ t) and 98.2% of Cr(VI) was removed within 60 min under the optimized conditions. According to the results of XPS with ion sputtering, Cr(VI) was removed via multiple pathways including adsorption, reduction and co-precipitation. This work not only offers a scalable route for MOFs-derived IC-ME materials, but also provides mechanistic insights into Cr(VI) removal from the perspective of Fe(II) dynamics.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yijun Chen,Meina Cheng,Yundong Wang,Long Jin,Juanhong Li,Hailiang Yang,Sanjian Ma,Guoliang Dai,Zixia Lin,Xin Liu
Both the iron sludge and usage of H 2 O 2 restrict the promotion of the Fenton reaction. Herein, we proposed a hydrogen-accelerated oxygen reduction Fenton reaction system named MHORF-UiO-66(Zr) to try to solve the two problems under normal temperature and pressure. The active hydrogen, which is derived from H 2 catalyzed by the composite of Pd/UiO-66(Zr), could accelerate the reduction of Fe(III) and promote the electron transfer of two-electron oxygen reduction reaction to realize the self-generation of H 2 O 2 . And 45.9 mM of H 2 O 2 could be detected. As expected, 91 % of trimethoprim (TMP) could be degraded within 30 min in this system in the condition of 25 μM Fe(II), H 2 30 mL·min −1 , and Pd/UiO-66(Zr) 2g·L −1 , which was 2.94 times that of the control Fenton system. Based on these results, the feasibility of fundamentally achieving zero emission of iron sludge was successfully verified. It was confirmed that both the hydroxyl radical and singlet oxygen played the dominant roles during the reaction process through the analysis of electron spin resonance spectroscopy. After six reaction cycles, the removal efficiency of TMP could be maintained at least 94 %. It found that both the properties and morphology of this composite could remain based on the systematic characterization.
研究领域:
环境科学
·
化学工程
·
催化材料
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Environmental Science-Nano
·
2023
·Vol. 10
·期 8
·2066-2076
·
IF 7.3
Jiahui Zhou,Xuesong Li,Qiuying Yi,Zhiwei Wang
Heterogeneous Fenton-like processes based on Fe-based catalysts are effective technology to degrade emerging organic pollutants in water and wastewater such as tetracycline (TC). However, the kinetically limited redox cycling between Fe2+ and Fe3+ is still a persistent challenge for their widespread application. To address this issue, we designed a novel Fe-based catalyst by coating reduced iron powder (RIP) with ferroferric oxide nanoparticles (FONP@RIP) using a simple chemical co-precipitation method. The reduced iron could rapidly reduce Fe(III) to Fe(II) and accelerate the cycle of Fe(II)/Fe(III) in the heterogeneous Fenton-like system. Benefiting from the accelerated cycle of Fe(II)/Fe(III), TC could be efficiently degraded in the FONP@RIP/H2O2 system over a wide pH range of 3–6, with a removal efficiency of 94.5% within 60 min (TC0 = 150 ppm). The predominant reactive oxygen species were identified as ˙OH and HO2˙. Based on the identified intermediates, the possible pathway of TC degradation was deduced and the toxicity of pollutants could also be significantly reduced during the degradation process. Moreover, FONP@RIP exhibited stable catalytic performance during multiple cyclic tests with only a marginal loss of catalytic components. This study presents a new catalyst design strategy for heterogeneous Fenton-like processes, which provides a promising way for the degradation of residual antibiotics in water and wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ying Fang,Qianwen Liu,Yang Song,Hui Cai,Ying Yang,Zhaoguang Yang,Haipu Li
Dissolved Fe(II) widely exists in high-arsenic (high-As) groundwater, whose concentration (12–518 µM) is positively correlated with that of As(III). In order to realize the environmental-friendly and highly efficient in-situ simultaneous oxidation and adsorption of As(III) under anoxic conditions, peroxymonosulfate (PMS) was directly dosed into Fe(II)-rich high-As groundwater. Compared with hydrogen peroxide (88.2%) and peroxydisulfate (66.6%), the involvement of PMS gave the best As(III) removal efficiency of 98.8% after 1 min treatment, owing to the dual aspects of the best oxidation of As(III) and the best adsorption of As(V). During As(III) oxidation process, more SO 4 • − and 1 O 2 generated and unactivated PMS in Fe(II)-PMS process were responsible for the most efficient oxidation. During the enhanced As(V) adsorption process, the presence of PMS changed the structure of the in-situ formed Fe(III) colloid to provide more adsorption sites. Besides, the higher PMS concentration caused better As(III) oxidation, As(III) immobilization, and As(V) adsorption efficiencies. A wide range of Fe(II) (125–500 µM) coupled with PMS (244 µM) could immobilize more than 90% of As(III) ( C 0 = 1000 µg/L), and As(III) ranging from 0.2 mg/L to 2.0 mg/L also could be removed over 90% in Fe(II)-PMS process. The coexistence of HCO 3 – , Cl − , and humic acid slightly affected As(III) immobilization. Furthermore, after treatment, residual Fe ions concentration, residual total arsenic concentration, sulfate ions concentration, and pH value met the drinking water standard. This study could provide a very promising and attractive technology for a fast and efficient in-situ purification of Fe(II)-rich high-As groundwater.
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WATER RESEARCH
·
2023
·
IF 12.8
Bin Liu,Yin Jun,Changrong Zhao,Chu Zhou,Tingting Zhu,Senlin Shao
Ultrafiltration (UF) is a technology commonly used to treat secondary effluents in wastewater reuse; however, it faces two main challenges: 1) membrane fouling and 2) inadequate nitrogen (N), phosphorus (P), and organic micropollutants (OMPs) removal. To address these two issues, in this study, we applied peracetic acid (PAA), Fe(VI)/PAA, and Fe(II)/PAA as UF pretreatments. The results showed that the most effective pretreatment was Fe(II)/200 μM PAA, which reduced the total fouling resistance by 90.2%. In comparison, the reduction was only 29.7% with 200 μM PAA alone and 64.3% with Fe(VI)/200 μM PAA. Fe(II)/200 μM PAA could effectively remove fluorescent components and hydrophobic organics in effluent organic matter (EfOM), and enhance the repulsive force between foulants and membrane (according to XDLVO analysis), and consequently, mitigate pore blocking and delay cake layer formation. Regarding pollutant removal, Fe(II)/200 μM PAA effectively degraded OMPs (>85%) and improved P removal by 58.2% via in-situ Fe(Ⅲ) co-precipitation. The quencher and probe experiments indicated that Fe IV O 2+ , •OH, and CH 3 C(O)OO•/CH 3 C(O)O• all played important roles in micropollutant degradation with Fe(II)/PAA. Interestingly, PAA oxidation produced highly biodegradable products such as acetic acid, which significantly elevated the BOD 5 level and increased the BOD 5 /total nitrogen (BOD 5 /TN) ratio from 0.8 to 8.6, benefiting N removal with subsequent denitrification. Overall, the Fe(II)/PAA process exhibits great potential as a UF pretreatment to control membrane fouling and improve water quality during secondary effluent treatment.
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CHEMOSPHERE
·
2021
·
IF 7.086
Peipei Huang,Lili Yao,Qing Chang,Yunhan Sha,Guodong Jiang,Shenghua Zhang,Zhe Li
The slow redox rate of Fe(III)/Fe(II) couples is a rate-limiting step for Fenton-like performance of Fe-MOFs. In this study, a series of catalysts (MIL-101) with various p-phthalic acid/2-aminoterephthalic acid (H 2 BDC/NH 2 –H 2 BDC) molar ratios were prepared using a simple and mild chemical method and applied for catalyzed degradation of bisphenol A (BPA). Interestingly, the –NH 2 modified MIL-101(Fe) can adjust Fe-Oxo node by increasing the electron density of Fe(III) in the presence of –NH 2 group with high electron density, thus forming Fe(II) in situ in MOFs. Meanwhile, the –NH 2 groups used as electron-donors can promote electron transfer , resulting in faster Fe(III)→Fe(II) half-reaction and active H 2 O 2 to continuously generate •OH radical. The BPA degradation and rate constant of Fe-BDC-NH 2 /H 2 O 2 system are 15.4-fold and 86.8-fold higher than that of Fe-BDC/H 2 O 2 system, respectively. The density functional theory (DFT) calculations showed that Fe-BDC-NH 2 possesses higher Fermi level energy (−4.88 eV) and lower activation energy barriers (0.32 eV) compared with Fe-BDC. Moreover, Fe-BDC-NH 2 showed good reusability and stability. This work offers a highly efficient and stable MOFs-based Fenton-like catalyst to rapidly degrade organic pollutants over a wide pH range for potential applications in wastewater treatment .
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