CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jialong Yin,Heng Zhang,Mengfan Luo,Jia Zhao,Bingkun Huang,Pinji Chen,Zhenpeng Cai,Yue Yuan,Yang Liu,Chuanshu He,Bo Lai
The ferrous species (Fe(II))-periodate (PI) system employs efficient decontamination by generating ferryl species (Fe(IV)-oxo) under acidic pH conditions. However, the mechanisms by which the Fe(II)/PI system operates across a broad pH range remain elusive. In light of the rapid oxidation and consumption of Fe(II) at neutral pH, we developed an electro-Fe(II) system utilizing an iron plate anode to activate PI (E(Fe/C)/PI). Efficient sulfamethoxazole (SMX) degradation was achieved under the E(Fe/C)/PI system across a range of pH values. Quenching and chemical probe experiments revealed a transition from Fe(IV)-oxo to singlet oxygen ( 1 O 2 ) as the predominant reactive species from acidic to near-neutral pH, respectively. Density functional theory (DFT) calculations indicated that the differences in one-electron transfer capacity and hydrolysis pathways for various protonated Fe(IV)-oxo species underlie the variations in catalytic mechanisms. This study not only enhances the efficiency of the Fe(II)/PI system but also provides a comprehensive understanding of the activation mechanisms at different pH levels.
研究领域:
环境化学
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电化学
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催化
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水处理
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产品关联
DOI
高影响因子
CHEMICAL GEOLOGY
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2025
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IF 3.6
Changjin Liang,Honghai Wu,Yaowei Li,Yufeng Guan
Ferrihydrite (Fh) can usually transform into phases with higher crystallinities. This may greatly alter Fh adsorption capacity for chromium ions, thereby affecting their immobilizations and fates. Foreign elements [e.g., lanthanum (La)] as impurities can become incorporated into Fh. Herein, the effect of La-substitution into Fh and the influence of the presence of Cr(VI) on Fh phase transformation and fate of Cr(VI) were investigated. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Electro-chemical impedance spectroscopy (EIS), and X-ray photoelectron spectroscopy (XPS) and other test methods were employed to probe phase changes after the Fe(II)-induced La-substituted Fh (La-Fh) transformations. At pH 5.5, no neoformed phase was observed until 7 d for La-Fh or pure Fh at 1 mM Fe(II) aq, but all La-Fh systems underwent transformations at 5 mM Fe(II)aq. A low pH and Fe(II)aq level favored lepidocrocite (Lp) to form, whereas goethite (Gt) was the predominant phase rather than Lp as pH increased to 7.2 with higher level Fe(II)aq. However, the La-substitution inhibits the La-Fh transformation rate and path. This made 5 % La-Fh transformed to Lp after 30 d at pH 7.2 and 1 mM Fe(II)aq. The La-release was present to some extent during the transformation process. Either the inhibition to La-Fh transformation or the La-slow release favors the retention of early-adsorbed Cr(VI) on iron-mineral surface. The added Cr(VI) might promote the La-Fh transformation even under a lower-level Fe(II), primarily attributed to the rapid reduction of Cr(VI) to Cr(III) by Fe(II), which produced more liable Fe(III) in addition to the Cr(III) that can improve the mineral conductivity, thereby enhancing the La-Fh transformation. Mechanisms responsible for the Fe(II)-induced La-Fh transformation companying the La slow-release are proposed to provide insights into the reduction and immobilization of Cr(VI) under anaerobic conditions, thus demonstrating that La-Fh is a promising material for application in Cr-contaminated site remediation.
研究领域:
环境化学
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地球化学
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土壤科学
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材料科学
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环境修复
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 15
·6745-6757
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IF 2.7
Yingzi Lin,Ningning Sun,Qingyu Zhang,Lei Chen,Shengbo Sun,Hong Yang,Jing Chen,Qixuan Weng,Shuang Xue
To overcome the limitations of the Fe(II)-activated percarbonate process for ACT removal, this study introduced cysteine as a complexing agent into the Fe(II)/SPC system and enhanced the degradation efficiency of ACT. Investigations were conducted on the effects of pH, temperature, common anions (Cl−, HCO3− and NO3−) in the water column, and humic acid (HA) on the degrading efficiency of the Cys/Fe(II)/SPC system. The results showed that under ideal conditions, 99.9% removal of ACT at 0.05 mM could be achieved. Alkaline environments inhibited ACT degradation, whereas acidic environments promoted it. Electron paramagnetic resonance (EPR) successfully detected ˙OH and O2˙−, but no 1O2 radical signal was detected. Further research was carried out to determine how much ˙OH and O2˙− contributed to the oxidation process. The results showed that both ˙OH and O2˙− contributed to the degradation of the ACT, with ˙OH's contribution being particularly significant. Mass spectrometry analysis was used to determine the structure of the oxidation products. Vulnerable sites in ACT were predicted using density functional theory. Using LC-MS/MS analysis, seven intermediates of the Cys/Fe(II)/SPC degradation of ACT were individually identified. The results showed that the acetylamino group on ACT and the C–N bond on the benzene ring are susceptible to attack by ˙OH. The T.E.S.T. toxicity prediction model was used to predict the toxicity of ACT and its intermediates. The results showed a trend towards reduced acute toxicity and overall developmental toxicity.
研究领域:
环境科学
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水处理
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化学工程
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分析化学
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毒理学
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产品关联
DOI
高影响因子
Food Bioscience
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2019
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IF 3.22
Biao Yuan,Cong Zhao,Chen Cheng,De-chun Huang,Shu-jie Cheng,Chong-jiang Cao,Gui-tang Chen
Grifola frondosa protein was hydrolysed using Alcalase, and the resulting hydrolysates (CGFP) were filtered using 5 and 1 kDa nominal cut-off ultrafiltration membranes and separated using Sephadex gel chromatography . Two main fractions, named GFP-1 and GFP-2 were obtained. CGFP-Fe and GFP-Fe were synthesized using ferrous chelation. Results showed that the GFP-2 fraction with molecular weight of 963 Da had the highest Fe(II) chelating activity (2680 ± 40 μg/g). UV spectrum showed that the Fe(II) shifted the maximum absorption to shorter wavelengths. The peptides measured using FTIR showed that the GFP-Fe peptide and the un-chelated peptide had different C–O and C= O absorption peaks. The effects of CGFP, CGFP-Fe, GFP2-2 and GFP-Fe on splenocytes proliferation and cytokines secretion were studied in vitro . Both the GFP-2 and GFP-Fe had good immune-enhancing activity. Furthermore, GFP-Fe showed an ability to promote the proliferation of splenocytes and peritoneal macrophages. The iron-chelating peptide of Grifola frondosa still maintained its immune enhancing activity after in vitro gastrointestinal digestion. The results suggested that GFP-Fe might be beneficial as a new iron supplement and as an immunological enhancement .
研究领域:
生物化学
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免疫学
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营养学
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DOI
高影响因子
Journal of Materials Chemistry A
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2017
·Vol. 5
·期 36
·19378-19389
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IF 8.867
Yingpan Song,Fenghe Duan,Shuai Zhang,Jia-Yue Tian,Zhihong Zhang,Zhuo-Wei Wang,Chun-Sen Liu,Wen-Ming Xu,Miao Du
A series of nanocomposites comprised of iron oxide and mesoporous carbon (denoted as Fe3O4@mC) were derived from an Fe(II)-based metal–organic framework (525-MOF) by calcining at different temperatures. The advantages of chemical functionality, strong bioaffinity, and high stability of the Fe3O4@mC can be combined with the high specific surface area of 525-MOF leading to the formation of Fe3O4@mC nanocomposites as a scaffold for oxytetracycline (OTC) aptamer strands. The use of Fe3O4@mC nanocomposites reveals high OTC detection efficiency. The nanocomposite calcined at 900 °C (denoted as Fe3O4@mC900) is found to be the best candidate toward high-sensitivity and high-selectivity detection of OTC because of its excellent functionality, nanostructural properties, and high electrochemical performance. Accordingly, the Fe3O4@mC900-based electrochemical aptasensor displays high sensitivity with a low detection limit of 0.027 pg mL−1 within a broad linear range of OTC concentration from 0.005 to 1.0 ng mL−1. The aptasensor also exhibits high selectivity, reproducibility, stability, regenerability, and applicability in milk samples. All of these results indicate that the Fe3O4@mC nanocomposites that originated from 525-MOF can be applied in the fields of trace and fast antibiotic determination.
研究领域:
材料科学
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分析化学
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纳米技术
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环境科学
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食品安全
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Chenrui Liu,Yun Liu,Zhi Dang,Shuai Zeng,Chengcheng Li
In this paper, a kind of novel core-shell structured heterogeneous photo-Fenton catalyst, boron-doped reduced graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @B-rGO) composite, was successfully synthesized by heating the mixture of Borane-Tetrahydrofuran adduct and graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @GO) under reflux conditions. The core-shell structure of the catalyst had been confirmed by X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photo electron spectra (XPS), and electron energy loss spectrum (EELS). The experimental results for Bisphenol A (BPA) degradation demonstrated that the as-prepared catalyst exhibited much higher photo-Fenton catalytic activity than Fe 3 O 4 and reduced graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @rGO). Additionally, Fe 3 O 4 @B-rGO with mass concentration of doped boron at 9.3% exhibited the optimum catalytic property, in which system the BPA degradation kinetic rate constant was almost 1.96 times and 1.82 times of that in the systems with Fe 3 O 4 and Fe 3 O 4 @rGO, respectively. Finally, the mechanism analyses verified that OH, O 2 − and h + were the main reaction species in this system, and photo-electron generated by boron doped reduce graphene oxide (B-rGO) can accelerate the redox between Fe(II) and Fe(III). The excellent photo-Fenton performance, stability and magnetic separation properties make it promising for the degradation of organic compounds in waste water under visible light.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Hao Xu,Qian Ye,Jing Zhang,Qiansong Li,Meijing Wang,Peng Zhou,Guanyu Zhou,Qingguo Wang
In response to the inherent restriction of low Fe(II) regeneration in the Fenton process, this study demonstrated a mutual-promoting configuration, where oxygen functionalized g-C 3 N 4 (OCN) was applied in Fe(III)/H 2 O 2 system to utilize mild natural solar light (SL) for persistent Fe(II) generation. The constructed OCN/Fe(III)/H 2 O 2 /SL system exhibited strong adaptability to various pollutants, and it well outperformed the g-C 3 N 4 (GCN) modified system and the traditional Fenton system in pollutants degradation efficiency. Compared with GCN, OCN could significantly promote the Fe(II) generation under solar light (SL), leading to more efficient H 2 O 2 activation. The characterization analyses revealed the larger surface area and enhanced charge separation of OCN, which were considered to take main responsibility for its enhanced photoactivity. The complexation of Fe(III) with the carboxyl groups of OCN also benefited the Fe(II) generation. ·OH was detected as the dominant radical responsible for metronidazole (MNZ) degradation, and its production in the OCN modified system was about twice that in the GCN modified system and the Fenton system. Moreover, the precipitation of FeO x on the OCN surface benefited the charge separation of the OCN, so that the improved OCN enabled a slight enhancement of MNZ degradation in the reuse experiments. The intermediates of MNZ degradation were analyzed based on the results of LC-MS, which provided insight into MNZ degradation pathways. This work highlighted the concept of self-improving photocatalyst, the ingenious combination of photocatalysis and Fenton-like system formed a mutual-promoting situation where the OCN and the Fenton-like system could both be improved, which endowed the configuration great potential for green and economical oxidation in environmental remediation.
研究领域:
环境科学
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光催化
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水处理
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高级氧化过程
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DOI
PubMed
高影响因子
Advanced Healthcare Materials
·
2019
·Vol. 8
·期 23
·1900911
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IF 6.27
Peng Ji,Haiqin Huang,Shirui Yuan,Le Wang,Siqi Wang,Yiwei Chen,Na Feng,Hanitrarimalala Veroniaina,Ziheng Wu,Zhenghong Wu,Xiaole Qi
Reactive oxygen species (ROS)-mediated apoptosis is considered a crucial therapeutic mechanisms for artesunate (AS). As an Fe(II)-dependent drug, the anticancer effect of AS is often limited due to insufficient Fe(II) concentration in targeted cells. To overcome this problem, a recombinant apoferritin nanocarrier containing ferriferous oxide (M-HFn) is constructed to produce auxiliary exogenous Fe(II) when delivering AS to cancer cells. Here, the newly fabricated AS-loaded M-HFn nanoparticles (M-HFn@AS NPs) can significantly improve the tumor-specific targeting and intracellular uptake efficiency of AS in human cervical carcinoma cells. After being captured in the acidic cavity of endosomes, M-HFn@AS NPs can simultaneously release Fe(II) and allow AS to activate satisfactory ROS-mediated apoptosis. Furthermore, in vivo studies demonstrate that M-HFn@AS NPs can selectively accumulate in tumors to efficiently inhibit tumor growth. Thus, M-HFn@AS NPs are a promising system to enhance the therapeutic effect of Fe(II)-dependent drugs.
研究领域:
药学
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癌症研究
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纳米技术
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分子生物学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL GEOLOGY
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2019
·
IF 3.618
Ying Wang,Xiu Yuan,Xiaomin Li,Fangbai Li,Tongxu Liu
Cytochrome c ( c -Cyts), as a key protein involved in extracellular electron transfer , plays an important role in the microbial Fe(II)-oxidizing process. In this study, due to their similar structure with the outer membrane protein of microorganisms , the equine c -Cyts was employed as a model protein to examine the impact of different organic ligands on the redox kinetics between Fe(II) and c -Cyts using the rapid stopped-flow spectrometer. Our results suggest that the presence of organic ligands will significantly accelerate the reaction between c -Cyts and Fe(II), with reaction rates obtained in the following order: EDTA > citric acid (Cit) > NTA > malonic acid (Mal) > glycine amino acid (Gly) > acetate acid (Ace) > control. It was also found from the kinetic modeling results that the reduction rate of c -Cyts by Fe(II)-ligands was closely correlated to the complex constant between Fe(II) and each ligand, and the reduction rate constants of c -Cyts by Fe(II)L species (L represents “ligands”). Further analysis on the ligand structure indicates that the reaction rate constants are highly correlated with the complex constants of Fe(II)-ligand and the reduction rate constants of c -Cyts by Fe(II)L species ( k 3 ) for Group I (Gly, NTA, and EDTA) and Group II (Cit, Mal, and Ace). The results of midpoint potentials of all Fe(II)-ligands obtained through cyclic voltammetry (CV) experiments were ranked as Ace < Gly < NTA < control < Mal < EDTA < Cit, indicating that the redox potentials of Fe(II) complexes in the same group with similar structures were positively correlated with Fe(II)-ligand complex constants. The reorganization energy change of the electron-transfer reaction resulting from the different Fe(II)-ligand structures may contribute significantly more than does the Gibbs free energy (Δ G ) to the reaction kinetics of Fe(II)-ligand and c -Cyts.
研究领域:
生物化学
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电化学
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微生物学
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蛋白质化学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Lingjie Liu,Shaoqing Mo,Shaopo Wang,Jing Chang,Jianhui Zhao,Jingjie Yu
Low temperatures were a critical factor that inhibited anaerobic ammonium oxidizing bacteria (AnAOB) activity. This study demonstrated the effect of exogenous zero-valent iron (ZVI) on Anammox-hydroxyapatite (HAP) system at 17°C. The results showed that long-term addition of ZVI increased the system nitrogen removal efficiency by 8.59% and alleviated the inhibition of AnAOB by low temperature. After addition of ZVI, the activity of AnAOB and the heme c content increased by 58.20% and 4.83%, respectively. Moreover, the functional enzyme activities of NIR, HZS, and HZO increased by 94.12%, 36.36%, and 16.67%, respectively. The concentrations of quorum sensing molecules, i.e., C 6 -HSL and C 8 -HSL, increased by 191.17% and 41.54%, respectively, after ZVI addition. Metagenomic analysis revealed that the addition of 5 g/L ZVI stimulated the relative abundance relative abundance of Fe(II) metabolism-related genes in AnAOB at 17 °C, thereby contributing to the uptake, transport, utilization, and storage of Fe(II). The addition of ZVI could improve the nitrogen removal performance of the anammox-HAP system at the low temperature.
研究领域:
环境工程
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微生物学
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生物技术
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产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Kunjie Hou,Zhoujie Pi,Fei Chen,Li He,Fubing Yao,Shengjie Chen,Xiaoming Li,Haoran Dong,Qi Yang
The practical application of the traditional Fenton system (Fe(II)/H2O2) is seriously hampered by the sluggish Fe(III)/Fe(II) cycle and the stringent acidic reaction condition. In this work, we found that trace-dissolved S(-II) (DS(-II), 5 μM) could significantly accelerate the Fe(III)/Fe(II) cycle and trigger a rapid H2O2 activation process in the Fe(III)/H2O2 system. Thus, more hydroxyl radicals (·OH) were generated for the rapid removal of various organic pollutants such as bisphenol A (BPA) and sulfamethoxazole (SMX) from water. Besides, the additive DS(-II) effectively broadened the application pH range of the Fenton or Fenton-like system. The constructed Fe(III)/DS(-II)/H2O2 system showed extensive applicability to different water matrices and maintained high BPA removal in the actual water sources. Furthermore, the toxicity assessment revealed that the toxicity of the target contaminant was diminished. The harmless SO42– was the final product of DS(-II) in the Fe(III)/DS(-II)/H2O2 system, and the residual DS(-II) was less than the threshold limit value for fresh or saltwater (0.5 mg/L). This discovery is expected to promote the large-scale practical application of iron-based Fenton or Fenton-like systems in practical organic wastewater purification.
研究领域:
环境科学
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水处理
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污染控制
✓ 已验证
DOI
Journal of Environmental Sciences
·
2023
·
IF 6.9
Ting He,Jie Sun,Liangwei Deng,Jialin Ming,Changwei Hu
Due to its high efficiency, Fe(II)-based catalytic oxidation has been one of the most popular types of technology for treating growing organic pollutants. A lot of chemical Fe sludge along with various refractory pollutants was concomitantly produced, which may cause secondary environmental problems without proper disposal. We here innovatively proposed an effective method of achieving zero Fe sludge, reusing Fe resources (Fe recovery = 100%) and advancing organics removal (final TOC removal > 70%) simultaneously, based on the in situ formation of magnetic Ca-Fe layered double hydroxide (Fe 3 O 4 @CaFe-LDH) nano-material. Cations (Ca 2+ and Fe 3+ ) concentration (≥ 30 mmol/L) and their molar ratio (Ca:Fe ≥ 1.75) were crucial to the success of the method. Extrinsic nano Fe 3 O 4 was designed to be involved in the Fe(II)-catalytic wastewater treatment process, and was modified by oxidation intermediates/products (especially those with COO − structure), which promoted the co-precipitation of Ca 2+ (originated from Ca(OH) 2 added after oxidation process) and by-produced Fe 3+ cations on its surface to in situ generate core-shell Fe 3 O 4 @CaFe-LDH. The oxidation products were further removed during Fe 3 O 4 @CaFe-LDH material formation via intercalation and adsorption. This method was applicable to many kinds of organic wastewater, such as bisphenol A, methyl orange, humics, and biogas slurry. The prepared magnetic and hierarchical CaFe-LDH nanocomposite material showed comparable application performance to the recently reported CaFe-LDHs. This work provides a new strategy for efficiently enhancing the efficiency and economy of Fe(II)-catalyzed oxidative wastewater treatment by producing high value-added LDHs materials.
研究领域:
环境工程
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废水处理
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）