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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Removal of acetaminophen in the Fe2+/persulfate system: Kinetic model and degradation pathways

Songlin Wang,Junfeng Wu,Xiuqing Lu,Wenxin Xu,Qing Gong,Jiaqi Ding,Bingsong Dan,Pengchao Xie

In this study, the removal of acetaminophen (ACT) in the Fe 2+ /persulfate system has been comprehensively evaluated. A kinetic model has been established based on the principal reactions. Good accordance between the experimental data and the predicted results under different operational conditions including molar ratio of Fe 2+ to persulfate, initial pH, initial ACT concentration, the presence of chloride, under natural water matrices and the mixture of ACT, amoxicillin and pyridine, evidences the validity of the proposed kinetic model. The rate constants for ACT reacting with SO 4 − and HO were determined as (1.80 ± 0.17) × 10 9  M −1  s −1 and (3.26 ± 0.41) × 10 9  M −1  s −1 , respectively. SO 4 − was evidenced to be the primary radical accounting for ACT removal through both kinetic model calculation and the scavenging results, using either methanol or tert -butyl alcohol. The optimum molar ratio of Fe 2+ to persulfate for ACT removal was determined to be 5:4. The removal rate of ACT was little affected by initial pH due to the rapid decrease of solution pH caused by the hydrolysis of iron ions. Cl − has a dual effect on the removal of ACT, and Cl 2 − rather than SO 4 − is proposed as the dominant radical for ACT removal at 10.0 mM Cl − . Possible degradation pathways are also proposed based on the detected intermediates.

研究领域: 环境科学 · 化学工程
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Polymer Chemistry · 2020 ·Vol. 11 ·期 37 ·6066-6072 · IF 5.342

A novel coumarin-chitosan fluorescent hydrogel for the selective identification of Fe2+ in aqueous systems

Shuangyu Xiong,Lian Duan,Xinjian Cheng

Some new chitosan-based fluorescent hydrogels have been successfully prepared by grafting coumarin derivatives onto chitosan via a Schiff base forming reaction or acid amine condensation reaction. It is worth noting that hydrogels synthesized by the Schiff base forming reaction can be used as a good fluorescent sensor for the selective recognition, detection and adsorption of Fe2+ ions in aqueous solution. Among them, the adsorption efficiency of 1 g of a fluorescent hydrogel to Fe2+ ions can reach 63.2 mg. In addition, after being further modified, hydrogels still retain the ability to identify and adsorb Fe2+. Therefore, this probe optimizes the synthetic route to chitosan-based fluorescent sensors and expands the practical application value of fluorescent hydrogels.

研究领域: 材料科学 · 环境科学 · 分析化学
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EUROPEAN POLYMER JOURNAL · 2021 · IF 4.598

Novel water soluble polymeric sensors for the sensitive and selective recognition of Fe3+/Fe2+ in aqueous media

Suyan He,Luminita Marin,Xinjian Cheng

Fe 3+ and Fe 2+ are common metal ions in natural water environments and creatures. The development of water-soluble fluorescent sensors for detecting Fe 2+ /Fe 3+ ions was of great significance. In this work, two kinds of boron fluoride dipyrrole (BODIPY) fluorescent small-molecules were synthesized firstly. One of the small molecules contains a thioester bond that can be used as a chain transfer agent to participate in the polymerization process, and the other contains an unsaturated C = C double bond at the meso position. Through the reversible addition-fragmentation chain transfer polymerization (RAFT) polymerization method, methacrylic acid (MAA) and methacrylamide (MAM) were used as the main monomers, and small molecular fluorescent monomers were introduced to the end of the main chain. In this way, fluorescent macromolecules were obtained. The polymers were water soluble owing to the presence of long enough hydrophilic carboxyl and amide chains. These fluorescent probes exhibit high sensitivity to Fe 2+ /Fe 3+ , good selectivity, and anti-interference of other ions. The detection limit for Fe 2+ was as low as 2.3 × 10 −7 M, and the detection limit for Fe 3+ can reach up to 4.5 × 10 −7 M. The results show that these probes can be used as good sensors to identify Fe 2+ and Fe 3+ . Moreover, the fluorophores could be incorporated into polymer chains as the RAFT reagents and/or functional monomers.

研究领域: 化学 · 材料科学
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JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING · 2022 · IF 5.168

The effect of the structure of functional monomers on the resistance of copolymers to Fe2+ and S2-

Chunyuan Wu,Haikuan Dong,Gaoshen Su,Huan Yang,Xiaorong Yu

Free radical solution polymerization method was used to preparing copolymers (FAPAM, IAPAM, and MAPAM) by copolymerizing acrylamide (AM) with functional monomers fumaric acid (FA), itaconic acid (IA) and maleic anhydride (MAH) respectively. The basic parameters of the polymer were characterized by fourier transform infrared spectrometer (FTIR), proton nuclear magnetic resonance spectroscopy ( 1 HNMR), elemental analyzer and ubbelohde viscometer . In polymer flooding , the viscosity reduction effect of Fe 2+ and S 2− in formation water is more serious than that of inert cations, and they have greater impact on oil recovery. Therefore, this paper studied the influence of functional monomers on the structure of polymers and the influence on the resistance to Fe 2+ and S 2− properties of polymers through rheometer , gel permeation chromatography (GPC) and scanning electron microscope (SEM). The results revealed that the intra-chain or interchain forces can be increased to varying degrees by introducing different functional groups into the polymer molecular chains , as a result, the copolymer had different resistance to Fe 2+ and S 2− . In addition, the carboxyl groups on MAPAM chain were the most evenly distributed, its configuration was the most regular, and its resistance to Fe 2+ was the strongest. Relatively, the carboxyl groups on IAPAM macromolecular chain were evenly distributed on both sides of the main chain, and it had the strongest ability to resist S 2− . The results of GPC and SEM further proved that the copolymers had the ability to resist Fe 2+ and S 2− .

研究领域: 化学工程 · 材料科学
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APPLIED ORGANOMETALLIC CHEMISTRY · 2023 ·Vol. 37 ·期 8 ·e7143 · IF 3.9

Complementarity and action mechanisms of Fe2+-activated persulfate and H2O2 system

Bolun Yu,Jingjing Yao,Haipu Li,Hui Ying Yang

The Fe 2+ -activated persulfate and H 2 O 2 (Fe 2+ /persulfate/H 2 O 2 ) system achieved 94% removal of four mixed sulfonamides with 300-s treatment and possessed excellent complementarity and stability over a wide pH (3–11) and temperature (5–65°C) range. The quenching and electron spin resonance spectroscopy results confirmed the coexistence of sulfate radicals and hydroxyl radicals in the coupled system, which were responsible for the elimination of sulfonamides under ambient conditions. The reaction rate constants of sulfate radicals and hydroxyl radicals at possible reactive sites distinguished the difference in removal ratios of four sulfonamides, according to experimental determination and density functional theory calculations. The removal ratio of sulfathiazole was higher than others because its calculated reaction rate constants of sulfate radicals and hydroxyl radicals were higher than those of sulfamerazine, sulfamethoxazole, and sulfamethazine. The finding provided a reference for investigating the removal mechanism of mixed organic pollutants in the presence of multiple free radicals.

研究领域: 环境科学 · 化学
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Journal of Physical Chemistry C · 2023 · IF 3.7

High-Yield, Stable, and Ultrasensitive Carbon Dots for pH Sensing and Fe2+ Detection Are Synthesized at Room Temperature

Chunyu Yu,Xue Li,Xin Qiao,Zhiwei Zhang,Danyang Zhang,Hua Liu,Xue-Li Hao,Zhongzhi Wang,Hongpeng You,Liang Zhou

Fluorescent carbon quantum dots (r-CDs) were synthesized safely and readily by stirring at room temperature with a yield of 76.5%. The synthesized r-CDs exhibit bright green emission with an absolute quantum yield of 12.0% under the excitation of ultraviolet light. Within the pH range of 3–12, the r-CDs exhibit excellent fluorescence stability. Interestingly, the fluorescence intensity of r-CDs faded promptly when the pH value diminished to 2 and then regained when the pH value returned to 3. This means that r-CDs can be used as “on–off–on” fluorescent probes for pH sensing. The mechanism of this sensitive pH response behavior was discussed in detail, and a possible mechanism of protonation–deprotonation–protonation processes was proposed. In addition, we have proposed a green preparation route for eco-friendly filter paper using anticounterfeiting. Interestingly, the presence of Fe2+ significantly quenched the fluorescence of r-CDs. Experimental results demonstrated the r-CDs can also be used to detect the content of Fe2+ in water, and the detection limit was 8.82 μM/L.

CAS / MDL: 10043-52-4 543-90-8
研究领域: 化学 · 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Enhanced removal of Microcystis aeruginosa in BDD-CF electrochemical system by simple addition of Fe2+

Yujiao Long,Hongna Li,Xuan Xing,Jinren Ni

This study presented a significant enhanced removal of Microcystis aeruginosa by simple addition of Fe 2+ at circumneutral pH in the electrochemical system with boron-doped diamond (BDD) anode and carbon felt (CF) cathode. Results showed that over 99.9% of the M. aeruginosa cells were removed in 60   min when 0.2   mM Fe 2+ was added to the system. The pseudo-first order rate constant for BDD-CF-Fe 2+ system was almost 15 times higher than that (0.005   min −1 ) for BDD-CF system. The excellent performance of the BDD-CF-Fe 2+ system over the BDD-CF system was observed over a wide range of pH from 3 to 9. Based on the evolution of Fe 2+ /Fe 3+ , pH, H 2 O 2 and OH, mechanism of enhanced removal of M. aeruginosa was revealed in the BDD-CF-Fe 2+ system. H 2 O 2 was electrochemically generated through reduction of dissolved oxygen on the surface of the CF cathode, and the added Fe 2+ was rapidly adsorbed and precipitated also on the CF cathode. Comparisons of BDD-CF-Fe 2+ , BDD-CF-Fe 3+ and BDD-CF-Fe 2+ /Fe 3+ systems proved that the electrochemical reduction of Fe(III) to Fe(II) could guarantee the sustainable cycle between Fe(II) and Fe(III). Through heterogeneous electro-Fenton reactions, much higher amount of OH would be continuously generated compared with the BDD-CF system. Thereby, the lipid peroxidation on the cell membrane of M. aeruginosa was intensified through the addition of Fe 2+ . Moreover, the degradation of intracellular microcystin was remarkably accelerated, and the extracellular microcystin was controlled more safely due to Fe 2+ addition. This study provided an alternative method to enhance the electrochemical mitigation of cyanobacteria-polluted waters.

CAS / MDL: 5470-11-1 14402-67-6
研究领域: 环境科学 · 微生物学 · 水处理技术
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY · 2022 ·Vol. 414 ·期 23 ·6735-6741 · IF 4.478

Ratiometric fluorescence nanoprobe based on carbon dots and terephthalic acid for determining Fe2+ in environmental samples

Wang Huaxin,Fu Ting,Ai Mimi,Liu Jinshui

A ratiometric fluorescent nanoprobe using carbon dots (CDs) and involving oxidation of terephthalic acid (TPA) induced by hydroxyl radicals (·OH) was developed for sensitively and selectively determining Fe 2+ ions. When Fe 2+ ions are added to the TPA@CDs/H 2 O 2 system, ·OH produced through the Fenton reaction oxidizes the non-fluorescent TPA to give 2-hydroxyl terephthalic acid, which fluoresces at 423 nm when excited at 286 nm. The ·OH and Fe 3+ produced quench CD fluorescence at 326 nm. The 2-hydroxyl terephthalic acid to CD fluorescence intensity ratio linearly increased as the Fe 2+ concentration increased in the range 0.5–50 μM, and the detection limit was 0.25 μM. The new assay is very selective because it involves dual-emission reverse change ratio fluorescence sensing, which can exclude matrix effects. The new nanoprobe was used to determine Fe 2+ concentrations in real water samples, and the recoveries were found to be acceptable. Graphical abstract Schematic of the ratiometric fluorometric method for determining Fe 2+ based on CDs and TPA

研究领域: 分析化学 · 环境科学
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TALANTA · 2018 · IF 4.244

N-doped carbon dots/H2O2 chemiluminescence system for selective detection of Fe2+ ion in environmental samples

Syed Niaz Ali Shah,Xiangnan Dou,Mashooq Khan,Katsumi Uchiyama,Jin-Ming Lin

The nitrogen doped carbon dots (N-CDs) produces strong chemiluminescence (CL)-emission due to hydroxyl radical ( • OH) induced electron-hole transition in N-CDs. The Fe 2+ has the ability to generate • OH from available hydrogen peroxide (H 2 O 2 ). Therefore, a pre-mixed N-CDs/H 2 O 2 solution was utilized for selective quantification of Fe 2+ in solution via CL-emission. A linear increase in the CL-emission intensity was observed within increase in Fe 2+ concentration. The N-CDs/H 2 O 2 system enabled the detection of Fe 2+ up to lower concentration of 0.2 × 10 −9 M with a linear dynamic range of 1.0 × 10 −9 –1.0 × 10 −6 M. Significantly, no CL-emission was observed when other divalent cations , Al 3+ , Fe 3+ , or Cr 3+ were injected to this system. Moreover, no interference was observed when a mixed solution of Fe 2+ and other cations were introduced to N-CDs/H 2 O 2 . The practical evaluation of N-CDs/H 2 O 2 system was demonstrated for detection of Fe 2+ in tap, lotus pond, and canal water samples. The easy detection, high sensitivity, and selectivity make this method a significant tool for analysis of Fe 2+ in solution.

CAS / MDL: 10049-05-5
研究领域: 分析化学 · 环境科学
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RSC Advances · 2019 ·Vol. 9 ·期 57 ·33017-33022 · IF 3.049

Fe2+ doped in CsPbCl3 perovskite nanocrystals: impact on the luminescence and magnetic properties

Yue Hu,Xinyue Zhang,Chaoqun Yang,Ji Li,Li Wang

All inorganic halide perovskite nanocrystals (NCs) have wider practical applications owing to their good properties, whereas the photoluminescence quantum yield (PLQY) of the purple emissive CsPbCl3 NCs is too low to apply in multi-color displays. In this study, earth-abundant Fe2+ metal ions were successfully incorporated into the lattice of CsPbCl3 NCs with the partial replacement of the sites of Pb2+ ions. The impacts of Fe2+ ions on the luminescence and magnetic properties of CsPbCl3 NCs were studied using photoluminescence spectroscopy (PL), X-ray diffraction spectroscopy (XRD), transmission electron microscopy (TEM), field emission scanning electron microscopy (FE-SEM), and a vibrating sample magnetometer (VSM). CsPb1−xFexCl3 NCs, with x = 0, 0.1, 0.2, and 0.3, were synthesized at 170 °C. It was found that an appropriate amount of Fe2+ doping not only improved the homogeneity of the size of NCs, but also enhanced the PLQY and average PL lifetimes. An obvious hysteresis behavior was observed for the NCs, and there was a significant change in the saturation magnetization value with the increase in the Fe2+ concentration.

研究领域: 材料科学 · 光学 · 磁学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Improving sewage sludge dewaterability with rapid and cost-effective in-situ generation of Fe2+ combined with oxidants

Jialin Liang,Siwei Zhang,Maoyou Ye,Jinjia Huang,Xian Yang,Shoupeng Li,Shaosong Huang,Shuiyu Sun

Zero-valent iron (ZVI) combined with oxidants is a promising conditioning strategy for improving sewage sludge dewaterability. However, challenges, such as a low dewatering rate and utilization efficiencies of ZVI, restrict further application of ZVI/oxidant treatments. This study employs, for the first time, rapid and cost-effective in-situ generation of Fe 2+ combined with common oxidants, namely H 2 O 2 , Na 2 S 2 O 8 , and KMnO 4 , to effectively improve sludge dewaterability. A comparative investigation of a standalone ZVI/oxidants treatment and when combined with a thermal and acid-wash (TA) pretreatment (TA/ZVI/oxidants) was systematically conducted to determine the sludge dewatering efficiency. Under the optimal operational conditions, the average water content of dewatered cake (Wc) was 18.47% less with the TA/ZVI/oxidants treatment when compared with the ZVI/oxidants treatment. The Wc values decreased to 54.81, 58.06, and 59.32 wt%, after the TA/ZVI/H 2 O 2 , TA/ZVI/Na 2 S 2 O 8 , and TA/ZVI/KMnO 4 treatments, respectively. The potential mechanism by which the TA/ZVI/oxidants treatment enhanced dewatering was investigated by determining the characteristics of both the sludge and the ZVI surface structure. Results indicate that the TA/ZVI/oxidants process caused more Fe 2+ dissolution, more strong oxidizing radicals and more strong flocculating Fe 3+ . The large amount of strong oxidizing radicals and strong flocculating Fe 3+ caused cell lysis and disrupted the protein-like and polysaccharide-like materials in the EPS, thereby decreasing the particle size, negative zeta potential, viscosity and colloidal forces, which then released the bound water trapped within the net-like floc and led to improved sludge dewaterability. In the ZVI reuse experiment, the TA/ZVI/oxidants treatment remained highly effective for sludge dewatering even after four cycles. Furthermore, economic analysis indicates that the TA/ZVI/H 2 O 2 treatment can save approximately 52.32% per year compared with using the traditional polyacrylamide (PAM) treatment.

研究领域: 环境工程 · 污水处理
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CRYSTENGCOMM · 2016 ·Vol. 18 ·期 37 ·7154-7162 · IF 3.849

Synthesis of composition and size controlled AuAg alloy nanocrystals via Fe2+-assisted citrate reduction

Yujiao Xiahou,Yijing Li,Peina Zhang,Lihui Huang,Dayang Wang,Haibing Xia

We report one new method for direct synthesis of monodisperse, quasi-spherical AuAg alloyed nanocrystals (ANCs) with sizes of 11 to 25 nm and core–shell (CS) AuAg@AuAg NCs (CS AuAg ANCs) with sizes of 30 to 80 nm via the Fe2+-assisted citrate coreduction of auric ions and silver ions in a one-pot reaction. It is found that at fixed concentration of auric ions, the concentrations of ferrous ions and silver ions play key roles in tuning the size and the types of NCs (AuAg ANCs and CS AuAg ANCs), respectively. Moreover, AuAg ANCs and CS AuAg ANCs exhibit excellent and poor chemical stability in nonideal chemical environments, respectively. The potential application of these AuAg ANCs for SERS detection of industrial pollutants (such as benzidine and p-cresol) in artificial industrial wastewater has been successfully demonstrated.

研究领域: 材料科学 · 纳米技术 · 环境科学
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