COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Zhongmin Feng,Jingwen Yang,Liangyuan Zhu,Ting Sun
Fe–based metal–organic frameworks (Fe–MOFs) have been widely used in heterogeneous Fenton-like processes. However, the catalytic performance of Fe-MOFs is limited by the relatively slow Fe (III)/Fe (II) redox cycle. For Fe-MOFs, increasing the interfacial electron transfer and reducing the electron density of Fe-MOFs are expected to accelerate the reduction of Fe (III) and improve the catalytic performance. Here, by mixing Fe/Cu metal species and introducing bromine groups, we successfully prepared bromine-functionalized bimetallic MOFs–FeCu(BDC-Br), and we used it to effectively degrade phenol in a Fenton-like process. Compared with most other catalysts, FeCu(BDC-Br) achieved a higher phenol degradation kinetic rate of 0.106 min –1 at a low dose. Effects of pH, humic acid (HA) and coexisting ions on the degradation of phenol were examined. The FeCu(BDC-Br) /H 2 O 2 system can remove phenol in the near neutral pH range of 4–6 and 0–50 mg/L HA range. Chloride ion , sulfate, or phosphate with a concentration of 100 mg/L showed an inhibitory effect on the catalytical performance of phenol degradation. This work provides insights for the preparation of Fe-MOFs Fenton-like catalyst in water/wastewater treatment.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
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IF 9.028
Shuchang Wang,Yang Deng,Binbin Shao,Jiahui Zhu,Zixin Hu,Xiaohong Guan
For the first time, this study showed that the apparent second-order rate constants (kapp) of six selected emerging organic contaminants (EOCs) oxidation by Fe(VI) increased, remained constant, or declined with time, depending on [EOC]0/[Fe(VI)]0, pH, and EOCs species. Employing excess caffeine as the quenching reagent for Fe(V) and Fe(IV), it was found that Fe(V)/Fe(IV) contributed to 20–30% of phenol and bisphenol F degradation by Fe(VI), and the contributions of Fe(V)/Fe(IV) remained nearly constant with time under all the tested conditions. However, the contributions of Fe(V)/Fe(IV) accounted for over 50% during the oxidation of sulfamethoxazole, bisphenol S, and iohexol by Fe(VI), and the variation trends of kapp of their degradation by Fe(VI) with time displayed three different patterns, which coincided with those of the contributions of Fe(V)/Fe(IV) to their decomposition with time. Results of the quenching experiments were validated by simulating the oxidation kinetic data of methyl phenyl sulfoxide by Fe(VI), which revealed that the variation trends of kapp with time were significantly determined by the change in the molar ratio of Fe(V) to Fe(VI) with time, highlighting the key role of Fe(V) in the oxidative process. This study provides comprehensive and insightful information on the roles of Fe(V)/Fe(IV) during EOC oxidation by Fe(VI).
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Peng Zhou,Xiaowei Huo,Jing Zhang,Yang Liu,Feng Cheng,Xin Cheng,Yunqi Wang,Yongli Zhang
Hydroxylated fullerene (fullerenol) has gained increasing attention in the field of water environment remediation based on its intrinsic properties of photosensitivity and high water solubility. In this work, C 60 fullerenol was added to the Fe(III)/PMS process to enhance diethyl phthalate (DEP) degradation both with and without visible light. The DEP removal ratio was increased from 2.2% to 58.8% with the addition of fullerenol at 60 min in dark condition, and the removal of DEP was completely achieved within 50 min under visible light irradiation. Mechanism investigation shows that carboxyl and carbonyl were formed via keto-enol isomerization at acid condition, resulting in the formation of open-cage fullerenol. The open-cage fullerenol can act as complex agent and electron donor to enhance oxidizing capability of the Fe(III)/PMS process by promoting Fe(III)/Fe(II) cycles. Competitive radical capture tests by electron spin resonance (ESR) and radical quenching analysis demonstrate that hydroxyl radical and sulfate radical were primarily responsible for DEP removal, but not superoxide radical and singlet oxygen. The DEP removal in the F/Fe(III)/PMS process is more efficiency at initial pH ranging from 2.1 to 4.9. Moreover, the DEP degradation route was proposed involving the generation of various intermediary products. This study provides a novel method for the application of fullerene derivatives on environment remediation by combining with metal catalyzed advanced oxidation processes.
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Journal of Cleaner Production
·
2024
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IF 9.7
Huihui Liu,Jiaying Yan,Yanlin Wu,Caixia Yan,Minghua Nie,Wenbo Dong
Sinapic acid (SA) as an environmentally friendly natural phenolic acid, has the properties of antioxidant because of containing –OH and –OCH 3 on the benzene ring and it is safe. The Fe(III)/peroxymonosulfate (PMS) system modified by SA for enhancing micropollutant degradation had been studied, while weather SA could improve micropollutant degradation in other Fe(III)/oxidants systems was still unclear. The Fe(III)/hydrogen peroxide (H 2 O 2 ) and Fe(III)/peroxydisulfate (PDS) systems modified by SA for micropollutants degradation were studied, the results indicated that SA could enhancing micropollutants degradation by accelerating the Fe(III)/Fe(II) cycle in both systems. In addition, the PMS, the H 2 O 2 and the PDS systems were compared, and ten micropollutants commonly present in natural water were selected to evaluate the oxidation capacity of different systems. The PMS and PDS systems have higher oxidation degradation capacity for ten micropollutants than that of H 2 O 2 system, attributed to the SO 4 •− , HO • and Fe(IV) all contributing to micropollutants degradation. However, in the H 2 O 2 system, ten micropollutants degradation almost entirely relied on HO • . In the PMS and PDS systems, the SO 4 •− played a dominated role for micropollutants removal, attributed to its higher steady-state concentration than HO • and its higher second-order reaction rate with micropollutants than Fe(IV). Economic evaluation indicted that the H 2 O 2 system was more cost-effective than the PMS and PDS systems for micropollutants removal. This was because the cost of H 2 O 2 was lower than PMS and PDS, and concentration of Fe(III), oxidants and SA requirements in the H 2 O 2 system were lower than that in the PMS and PDS systems. Overall, this study provided an economical and environmental-friendly method for the efficient treatment of harmful micropollutants in wastewater.
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Frontiers in Chemistry
·
2025
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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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ANALYTICAL CHEMISTRY
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2025
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IF 6.7
Kaixu Jin,Caipeng Xu,Yufen Zhao,Songsen Fu
Accurately determining the concentration and redox ratio of iron ions is crucial in fields such as biogeochemistry and environmental chemistry. While current NMR relaxometry-based methods are lauded for their simplicity and speed, they face challenges when paramagnetic matrices are present. This study overcomes this limitation by leveraging the redox sensitivity of iron ions. By using appropriate redox reagents and pH conditions, seamless transitions between Fe2+ and Fe3+ are achieved without altering the valence states of other common paramagnetic metals. The significant difference in the relaxometry rates of water protons induced by Fe2+ and Fe3+ enables a strong linear relationship across a concentration range of 0 to 500 μM, with a detection limit of less than 1 μM. The established standard curves were effectively applied to determine the redox ratio and total iron concentration in both artificial and real samples, validated by X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma-optical emission spectrometry (ICP-OES) analyses. Furthermore, the method demonstrates resistance to interference from common ligands, suggesting its promising potential for analyzing biological and food samples.
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JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 42
·19811-19824
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IF 3.5
Liu Weinan,Zhang Haiyang,Yuan Hang,Wang Lidong,Li Zhen
Peroxymonosulfate (PMS) is widely used in advanced oxidation processes. Fe(II) is an excellent catalyst for PMS, and organic pollutants in water can be effectively degraded in the Fe(II)/PMS system. However, the pollutant degradation efficiency is limited by the low conversion efficiency of Fe(II). Natural antioxidants exist in the water environment and have strong electron-donating ability. At present, the research on the introduction of natural antioxidants into the advanced oxidation processes to degrade pollutants focuses on a few polyphenols, and the effects of other natural antioxidants on the removal of pollutants are worth studying. In this study, natural antioxidants, proanthocyanidins (PCs), saponins (SPs), and Lycium barbarum polysaccharides (LBPs), were introduced into the Fe(III)/PMS system. The reduction ability of natural antioxidants was used to improve the conversion efficiency of Fe(III) to Fe(II), and PMS was more effectively activated to produce ROS, which promoted the degradation of ofloxacin (OFL). After the introduction of PC in the Fe(III)/PMS system, 80% of OFL was degraded at 20 min, and 90% of OFL was degraded at 120 min after the introduction of SP. The experimental results showed that the degradation of OFL was affected by the amount of antioxidants, PMS and Fe(III), pH value, and coexisting anions. Free radical quenching experiments showed that 1 O 2 , SO 4 − ·, and ·OH play an important role in the degradation of OFL in the Fe(III)/antioxidant/PMS system. This paper proves that the introduction of proanthocyanidins and saponins into the advanced oxidation processes can remove organic pollutants more efficiently. Graphical
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Huihui Liu,Jie Zhao,Yu Wang,Yanlin Wu,Wenbo Dong,Minghua Nie,Xiaoning Wang
Peroxymonosulfate (PMS) is more cost-effective than peroxydisulfate (PDS) and has drawn great attention presently. Low efficiency of Fe(III)/Fe(II) cycle is a great intrinsic drawback of Fenton-like system, which extremely limits its widespread application. In this study, sinapic acid (SA) as a natural and environmental-friendly reductant, was applied to enhance Fe(III)/Fe(II) cycle in PMS/Fe(III) system. The removal efficiency of methyl paraben (MEP) was 98.3% (7.2 × 10 −4 s −1 ) within 90 min in the modified system, and the k obs was 18 times higher than in PMS/Fe(II) system. For the active species identification, SO 4 − , HO and Fe(Ⅳ) were all responsible for MEP degradation, while SO 4 − was the dominant radical. The role of SA in SA/PMS/Fe(III) system was investigated, Fe(III) was reduced to Fe(II) and SA was oxidized to quinone species in this reaction process. The concentration of Fe(II) and the activation efficiency of PMS were all improved with SA concentration increasing from 5 to 20 μM, and the contribution of active species for MEP degradation were estimated. The effect of initial pH and common anions were also investigated. For the effect of anions, HCO 3 − and SO 4 2− presented inhibition effect on MEP removal, and with the HCO 3 − concentration increasing 1–10 mM the inhibition decreased. Low concentration Cl − promoted MEP degradation while Cl − with higher concentration exhibited inhibition. And NO 3 − was almost no effect on MEP degradation.
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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
·
催化材料
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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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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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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 26
·14793-14805
·
IF 12.732
Yuan Gao,Xiaoguang Duan,Bin Li,Qianqian Jia,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Shaobin Wang,Wenchao Peng
Persulfate-based advanced oxidation processes are promising technologies to solve water pollution. In this work, single iron atoms are anchored on three-dimensional N-doped carbon nanosheets by a chemical vapor deposition (CVD) method with ferrocene-loaded CaO as the hard template. The high surface density of Fe–N4 sites and abundant interconnected meso–macro pores are highly favorable for activating peroxymonosulfate (PMS) to produce superoxide radicals (O2˙−), giving rise to ultrahigh activity and excellent stability for pollutant degradation. Experiment and density functional theory (DFT) calculations reveal that Fe–N4 is the main active site, on which electrons transfer from C to Fe via the C–N–Fe bond to secure the low-valence state of Fe species for the redox process. This work proposes a new strategy for developing highly active single-atom materials by CVD and reveals mechanisms of PMS activation on single-atom activators.
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