ANALYTICAL CHEMISTRY
·
2025
·
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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DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 42
·19811-19824
·
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
·
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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高影响因子
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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高影响因子
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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PubMed
高影响因子
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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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yunqi Wang,Peng Zhou,Qingguo Wang,Xiaowei Huo,Xue Huang,Qian Ye,Hao Xu,Guanyu Zhou,Yuhang Liu,Jing Zhang
Hydroxylated fullerene, Fullerol, has applied in many areas because of its high electron affinity and antioxidant potential, while it was few used in wastewater treatment. In this study, the mechanism involved that Fullerol accelerated the regeneration of Fe(II) in the Fe(III)/H 2 O 2 system under dark condition, which was investigated with chloramphenicol (CAP) as a model pollutant. In Fullerol/Fe(III)/H 2 O 2 system, CAP removal was completely achieved at 60 min via a non-photochemical pathway. In addition, the quenching experiments and electron spin resonance (ESR) results indicated that hydroxyl radical ( OH) was the main reactive oxygen species (ROSs). The Fullerol/Fe(III)/H 2 O 2 system had a rate constant of CAP degradation about 5.0 × 10 −2 min −1 , which was about 22 times higher than it in Fe(III)/H 2 O 2 Fenton-like system (2.3 × 10 −3 min −1 ). Fe(II) was ascertained the effective component that was responsible for H 2 O 2 activation to produce OH, which derived from 1) the first pathway: Fullerol complexed with Fe(III) and the redox potential of the complex is much lower than Fe(III)/Fe(II); 2) the second pathway: Fullerol acted as an electron donor to reduce Fe(III) into Fe(II). Moreover, CAP degradation intermediates were identified and its degradation pathways were proposed. This study suggested a new approach for improving the Fe(III)/H 2 O 2 system by accelerating Fe(III)/Fe(II) cycles with Fullerol.
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Catalysts
·
2022
·Vol. 12
·期 11
·1435
·
IF 4.501
Fujian Yang,Cheng Yin,Mengqiao Zhang,Jiangwei Zhu,Xiuyuan Ai,Wenchao Shi,Guilong Peng
The activation of persulfate (PS) by Fe(III) for the removal of environmental organic pollutants was severely limited by the low reduction rate from Fe(III) to Fe(II). In present study, we reported that reducing sulfur species (i.e., SO32−, HSO3−, S2−, and HS−) under low concentration could significantly accelerate the Fe(III)/Fe(II) cycle in the Fe(III)/PS system. Under the condition of 1.0 mM Fe(III) and 4.0 mM PS, the removal performance of Fe(III)/PS system was poor, and only 21.6% of BPA was removed within 40 min. However, the degradation efficiency of BPA increased to 66.0%, 65.5%, 72.9% and 82.7% with the addition of 1.0 mM SO32−, HSO3−, S2−, and HS−, respectively. The degradation efficiency of BPA was highly dependent on solution pH and the concentration of reducing sulfur species. When the reductant was excessive, the removal efficiency would be significantly inhibited due to the elimination of reactive species. This study provided some valuable insights for the treatment of organic wastewater containing these inorganic reducing ions.Keywords:persulfate;reducing sulfur species;cycle;degradation
研究领域:
环境科学
·
化学
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高影响因子
CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Jie Liu,Chunmiao Liu,Yanchun Tong,Haibin Sun,Hui Peng,Mingwei Zhang,Shigang Wu,Hongying Zhang,Hongyu Gong,Zhiqin Zheng,Xue Guo,Yurun Feng
The SiCN/Fe/Ni ceramics codoped with iron acetylacetonate (FA) and nickle acetylacetonate (NA) was synthesized by polymer-derived ceramics (PDCs) method in this study. The microstructure, phase composition and electromagnetic wave (EMW) absorption properties of the samples were analyzed. The polarization loss and conduction loss of materials were analyzed by the direct current (DC) multimeter and the contribution rate of polarization loss was more than 94% in the whole frequency band. The results showed that C, SiC, Fe 2 Si, Ni 3 Si, γ- (Fe, Ni) and CNTs were formed after pyrolysis which provided lots of heterogeneous interface and enhanced the interfacial polarization. Meanwhile, Ni could enter the lattice of Fe and formed a unique electronic configuration, which reinforced the conductivity and stability of Fe. In addition, the in-situ generated Fe 2 Si and Ni 3 Si provided magnetic loss and conduction loss. The RL min value of SiCN/Fe/Ni-3 ceramic was −52.06 dB at 1.54 mm and the effective absorption band (EAB, RL ≤ −10 dB) reached 4.21 GHz (13.79–18 GHz, 1.43 mm).
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高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6
Zhengxi Zou,Zhenke Xu,Weiming Hua,Yinghong Yue,Zi Gao
Catalytic ethane dehydrogenation to ethylene is an attractive route for ethylene production following the shale gas revolution. However, its industrial implementation remains challenging due to high costs and environmental concerns. Iron-based catalysts have been identified as promising alternatives, while their catalytic performance is significantly dependent on the coordination environment and oxidation state of the iron species. Herein, a series of Fe/ZSM-5 catalysts were synthesized via urea precipitation (FeZ-P) and incipient wetness impregnation (FeZ-I) methods to investigate the relationship between Fe species evolution and catalytic behavior during ethane dehydrogenation. The FeZ-P catalysts exhibited significantly enhanced activity compared with FeZ-I, which was attributed to the improved dispersion of iron species and their favorable transformation behavior under reaction conditions. Detailed characterizations of fresh and spent catalysts revealed that the initial Fe 2 O 3 species on FeZ-P surface possessed limited dehydrogenation activity but underwent reaction-induced reduction and carbonization, generating Fe 3 C with enhanced ethane dehydrogenation performance. In contrast, the Fe 2 O 3 bulks on FeZ-I exhibited slower transformation rates, resulting in inferior catalytic activity. Air oxidation treatment enabled partial regeneration of the catalyst by removing carbon deposits and modifying Fe species evolution. This study highlights the importance of regulating Fe species dispersion and dynamic reduction-carbonization behavior, through which catalytically active Fe 3 C can be generated for enhanced ethane dehydrogenation performance. These findings provide valuable insights into the rational design of efficient Fe-based catalysts for non-oxidative alkane dehydrogenation.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Ning Gu,Yueyang Xu,Yan Yin,Xuzhao Gao,Yongping Zeng
SO x released from the combustion of sulfur-containing compounds in fuels pollute the environment and have a serious impact on human health. Adsorption desulfurization is an effective and environmentally friendly technique for removing sulfur-containing compounds from fuels. Metal-organic frameworks (MOFs) have high specific surface areas and can be easily modified and functionalized, making them excellent candidates for adsorption desulfurization in fuels. In this work, the precursor MIL-100(Fe)-SA was prepared using the hydrothermal method , and the adsorbent Ni@MIL-100(Fe)-SA was obtained by doping Ni 2+ into the resulting MIL-100(Fe)-SA using the impregnation method. FT-IR, X-ray diffraction, scanning electron microscopy, transmission electron microscopy and nitrogen adsorption-desorption isotherms were used to analyze the samples. The results indicated that Ni 2+ was successfully loaded onto MIL-100(Fe)-SA, and the MOF's structure remained stable. The adsorption performance of benzothiophene and thiophene was evaluated through batch adsorption experiments. The adsorption capacities of Ni@MIL-100(Fe)-SA for thiophene and benzothiophene were 23.68 mg S/g and 49.58 mg S/g, respectively. These observations could be ascribed to the π-complexation interactions between Ni 2+ of the framework and thiophenic compounds. The regeneration experiments demonstrated that the spent 11Ni@MIL-100(Fe)-SA-1.5 reach 86% of the adsorption capacity of fresh adsorbent after four cycles. Additionally, the regenerated adsorbent maintained good crystallinity after recycling.
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