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CHEMICAL PHYSICS LETTERS · 2017 · IF 1.815

CTAB induced emission from water soluble polyarylene ether nitrile carboxylate and selective sensing of Fe (III) ions

Shiliang Wei,Kun Jia,Hongguo Shou,Xuefei Zhou,Pan Wang,Xiaobo Liu

Polyarylene ether nitrile (PEN) is traditionally used as high performance thermoplastics in various advanced engineering materials fields. However, the preparation of optically active PEN based materials, especially in aqueous solution, is still a great challenge. In this work, the side chain carboxylated PEN can be readily dissolved in alkaline solution but showing strongly quenched luminescence. Fortunately, the cationic surfactant of cetyltrimethylammonium bromide (CTAB) was able to recover the fluorescence emission of water soluble PEN, which can be subsequently quenched by Fe 3+ ions, leading to the selective determination of Fe 3+ ions in aqueous solution.

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ENVIRONMENTAL POLLUTION · 2017 · IF 5.099

Microbial siderophores and root exudates enhanced goethite dissolution and Fe/As uptake by As-hyperaccumulator Pteris vittata

Xue Liu,Jing–Wei Fu,Evandro Da Silva,Xiao–Xia Shi,Yue Cao,Bala Rathinasabapathi,Yanshan Chen,Lena Q. Ma

Arsenic (As) in soils is often adsorbed on Fe-(hydro)oxides surface, rendering them more resistant to dissolution, which is undesirable for phytoremediation of As-contaminated soils. Arsenic hyperaccumulator Pteris vittata prefers to grow in calcareous soils where available Fe and As are low. To elucidate its mechanisms of acquiring Fe and As from insoluble sources in soils, we investigated dissolution of goethite with pre-adsorbed arsenate (AsV; As-goethite) in presence of four organic ligands, including two root exudates (oxalate and phytate, dominant in P. vittata ) and two microbial siderophores (PG12-siderophore and desferrioxamine B). Their presence increased As solubilization from As-goethite from 0.03 to 0.27–5.33 mg L −1 compared to the control. The siderophore/phytate bi-ligand treatment released 7.42 mg L −1 soluble Fe, which was 1.2-fold that of the sum of siderophore and phytate, showing a synergy in promoting As-goethite dissolution. In the ligand-mineral-plant system, siderophore/phytate was most effective in releasing As and Fe from As-goethite. Moreover, the continuous plant uptake induced more As-goethite dissolution. The continued release of As and Fe significantly enhanced their plant uptake (from 0.01 to 0.43 mg plant −1 As and 2.7–14.8 mg plant −1 Fe) and plant growth (from 1.2 to 3.1 g plant −1 fw) in P. vittata . Since microbial siderophores and root exudates often coexist in soil rhizosphere, their synergy in enhancing dissolution of insoluble As-Fe minerals may play an important role in efficient phytoremediation of As-contaminated soils.

CAS / MDL: 83-86-3 338-70-5
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Journal of Materials Chemistry A · 2017 ·Vol. 5 ·期 30 ·15797-15807 · IF 8.867

Luminescent Cd(II)–organic frameworks with chelating NH2 sites for selective detection of Fe(III) and antibiotics

Dan Zhao,Xiao-Hui Liu,Yue Zhao,Peng Wang,Yi Liu,Mohammad Azam,Saud I. Al-Resayes,Yi Lu,Wei-Yin Sun

Excess and deficiency of iron(III) and antibiotics from normal permissible limits will induce serious disorders, so their detection is important but challenging. In this work, by introducing a new amino triazole ligand N1-(4-(1H-1,2,4-triazole-1-yl)benzyl)-N1-(2-aminoethyl)ethane-1,2-diamine (L), a series of Cd(II)-based metal–organic frameworks (MOFs) [Cd3(BDC)3(DMF)2] (1), [Cd(L)(BDC)]2·2DMF·H2O (2), [NaCd2(L)(BDC)2.5]·9H2O (3), [Cd2(L)(2,6-NDC)2]·DMF·5H2O (4) and [Cd2(L)(BPDC)2]·DMF·9H2O (5) were synthesized. MOFs 1, 2 and 3 obtained under the same conditions with the same auxiliary ligand (H2BDC) but different amounts of alkali (NaOH) show distinct 3D, 1D and 3D framework structures, respectively, in which L and BDC2− exhibit varied coordination modes. 4 and 5 with 3D structures were isolated by using longer auxiliary ligands of 2,6-H2NDC and H2BPDC. The porosity and excellent fluorescence performance of 3, 4 and 5 make them potential luminescent sensors for Fe(III) and antibiotics. The results show that 3, 4 and 5 represent high sensitivity for the detection of Fe(III) ions with detection limits of 155 ppb for 3, 209 ppb for 4 and 297 ppb for 5 due to the existence of open channels and chelating NH2 sites. In addition, the strong emissions of 3, 4 and 5 can be quenched efficiently by trace amounts of NFs (nitrofurazone, NZF; nitrofurantoin, NFT; furazolidone, FZD) antibiotics even in the presence of other competing antibiotics such as β-lactams (penicillin, PCL). They are responsive to NZF with detection limits of 162 ppb for 3, 75 ppb for 4 and 60 ppb for 5.

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CELLULOSE · 2017 ·Vol. 24 ·期 6 ·2403-2413 · IF 3.417

Catalytic conversion of cellulose into polyols using carbon-nanotube-supported monometallic Pd and bimetallic Pd–Fe catalysts

Xu Siquan,Yan Xiaopei,Bu Quan,Xia Haian

A series of carbon nanotube (CNT)-supported monometallic Pd and bimetallic Pd–Fe catalysts were synthesized and employed for catalytic hydrogenolysis of cellulose into polyols, including hexitol, ethylene glycol (EG), 1,2-propanediol (1,2-PG), and glycerol (Gly). The physicochemical properties of the catalysts were characterized by nitrogen physical adsorption measurements, X-ray diffraction analysis, transmission electron microscopy, and X-ray photoelectron spectroscopy. The total yield of hexitol, EG, 1,2-PG, and Gly in hydrolytic hydrogenation of cellulose was 37, 55, and 53% for Pd/CNTs, Pd–Fe/CNTs (Pd:Fe = 1:1), and Pd–Fe/CNTs (Pd:Fe = 1:2), respectively. Addition of Fe to Pd significantly modified the physicochemical properties of the nanoparticles and their catalytic performance, especially regarding hexitol selectivity. The promoting effect of Fe, especially for hexitol selectivity, compared with the monometallic catalyst is due to the fact that incorporation of Fe may stabilize Pd 0 nanoparticles and lead to downshift of the d -band center of Pd metal nanoparticles by charge transfer from Fe to Pd. Recycling experimental results showed that leaching of Fe resulted in a significant decrease in the hexitol yield obtained using the Pd–Fe/CNTs after the first recycle, further demonstrating that Fe element plays a promoting role for hexitol formation.

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ChemCatChem · 2014 ·Vol. 7 ·期 3 ·441-449 · IF 5.044

Encapsulation of Heteropolyanion-Based Ionic Liquid within the Metal–Organic Framework MIL-100(Fe) for Biodiesel Production

Hui Wan,Chong Chen,Zuowang Wu,Yigen Que,Yu Feng,Wei Wang,Lei Wang,Guofeng Guan,Xiaoqin Liu

Graphical Be more active: A new strategy is proposed to construct the ionic liquid, polyoxometalate (POM), and metal–organic framework (MOF) composite. POM bridges the gap between the ionic liquid and the carrier (MOF); thus, the heteropolyanion-based ionic liquid can be encapsulated within the cages of MIL-100 (MIL=Materials of Institut Lavoisier) through anion exchange. The POM–ionic-liquid-functionalized MOF demonstrates high catalytic activity for the esterification of oleic acid with ethanol and is stable in the liquid-phase reaction, with no obvious leaching of the active component. A new strategy was proposed to construct the ionic liquid, polyoxometalate (POM), and metal–organic framework (MOF) composite. The POM-based MOF was synthesized by using the direct hydrothermal method. The sulfonic acid group-functionalized ionic liquid was used for further modification of the hybrid material to realize the encapsulation of the heteropolyanion-based ionic liquid within the cages of the MOF. The catalysts were characterized by using XRD, N 2 adsorption–desorption, FTIR, SEM, TEM, elemental analysis, and TGA. The results indicated that the heteropolyanion-based ionic liquid had been successfully encapsulated within the cages and the structure of MIL-100 (MIL=Materials of Institut Lavoisier) remained intact. The POM–ionic-liquid-functionalized MOF, with high content of the active component, had both Lewis and Brønsted acid sites, which led to high catalytic activity for the esterification of oleic acid with ethanol. The esterification reaction conditions were optimized by using response surface methodology (RSM), and the corresponding conversion of oleic acid reached 94.6 %. The catalyst could be easily recovered and reused six times without significant loss of activity.

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RSC Advances · 2015 ·Vol. 5 ·期 50 ·40094-40102 · IF 3.84

Reverse-phase high performance liquid chromatography separation of positional isomers on a MIL-53(Fe) packed column

Zhiming Yan,Wenmin Zhang,Jia Gao,Yifen Lin,Jianrong Li,Zian Lin,Lan Zhang

The application of the metal–organic framework (MOF) MIL-53(Fe) as a novel stationary phase for reverse-phase high performance liquid chromatography (HPLC) separation of positional isomers is described for the first time. Under the optimized conditions, baseline separation of xylene, dichlorobenzene, chlorotoluene and nitroaniline isomers was achieved on the MIL-53(Fe) packed column within a short time. The retention mechanisms of these isomers on the MIL-53(Fe) packed column were discussed in detail, and a typical reverse-phase behavior can describe the results. The thermodynamic characteristics of the HPLC separation of positional isomers were also evaluated. It was confirmed that the HPLC separation of positional isomers was controlled by the Gibbs free energy change (ΔG). In addition, reverse-phase HPLC separation of the tested isomers was also carried on MIL-53(Al, Cr) packed columns to investigate the influence of the metal centre of the MIL-53 framework on their chromatographic behaviors. The results showed that the MIL-53(Fe) packed column exhibited better separation performance than the MIL-53(Al, Cr) packed columns. Moreover, the MIL-53(Fe) packed column also gave efficient HPLC separation of alkylbenzene and naphthalene, aniline compounds and polycyclic aromatic hydrocarbons (PAHs). These successful applications suggest the potential of MIL-53(Fe) as a novel stationary phase for efficient reverse-phase HPLC separation.

CAS / MDL: 100-21-0
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JOURNAL OF MOLECULAR CATALYSIS B-ENZYMATIC · 2013 · IF 2.823

Discovery of a new Fe-type nitrile hydratase efficiently hydrating aliphatic and aromatic nitriles by genome mining

Xiaolin Pei,Lirong Yang,Gang Xu,Qiuyan Wang,Jianping Wu

Microbial nitrile hydratases (NHases) are important industrial catalysts to produce valuable amides. However, only some NHase genes have been reported and studied at the molecular level. In this study, we developed a genome mining method to discover Fe-type NHases from GenBank. The putative NHase gene from Pseudomonas putida F1 was cloned and functionally expressed in Escherichia coli BL21 (DE3) by assisting of a putative activator gene adjacent to β-subunit region. Three recombinant plasmids containing NHase gene or the activator gene were designed and constructed. Maximal enzyme activity was obtained when the structural and activator genes were transcribed as one unit in plasmid pCDFDuet-1 at 18   °C. However, the expressed product did not show any NHase activity when the downstream activator gene was ignored, and the product completely existed in insoluble inclusion body. The activator gene might be involved in protein folding of the α- and β-subunits of NHase. In addition, the Fe-type NHase exhibited broad substrate specificity. The enzyme can efficiently hydrate aromatic nitriles, such as 3-cyanopyridine, 4-cyanopyridine, and benzonitrile, asides from aliphatic nitriles preferentially. Therefore, the recombinant NHase shows potential applications in some amides preparation.

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CHROMATOGRAPHIA · 2024 · IF 1.2

Enantioseparations of the Six Basic Drugs by MIL-100(Fe)-Modified Open-Tubular Columns in Capillary Electrochromatography

Shao Xiaozhen,Xu Guangfu,Chen Jiaquan,Miao Pandeng,Yang Ke,Du Yingxiang,Yu Tao

Metal–organic frameworks (MOFs) have a wide range of applications in separation and analytical sciences due to their unique structures. MIL-100(Fe) was immobilized on the inner wall of the capillary column based on the immobilized cysteine (Cys)-triggered in situ growth (ICISG) strategy. By applying this column to capillary electrophoresis, a novel enantioselective separation system based on MIL-100(Fe) nanomaterial was established. By utilizing lactobionic acid (LA) as the chiral selector and optimizing the experimental conditions such as buffer pH, LA concentration and the methanol addition ratio, the CEC system demonstrated a significantly enhanced enantioseparation ability for six basic drugs. The modified capillary column was characterized by scanning electron microscope (SEM), energy-dispersive X-ray spectroscope (EDS) and X-ray diffractometer. The experimental results showed that MIL-100(Fe) was successfully grown on the inner wall of the capillary column. In the present study, the repeatability of the coated column was investigated and the relative standard deviations (RSDs) of the resolution and the migration time for intra-day, inter-day and inter-column were within 8%, proving the good repeatability of the coated column.

CAS / MDL: 919-30-2 111-30-8
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ELECTROCHIMICA ACTA · 2024 · IF 5.5

Enhanced electrochemical reduction of N2 to NH3 by interfacial engineering of biomass-derived Fe, Mo-bimetallic composite

Daming Feng,Lixue Zhou,Chang Liu,Hui Li,Yusheng Zhang,Yali Yao,Tianyi Ma

Electrocatalytic nitrogen reduction reaction (NRR) for the synthesis of ammonia (NH 3 ) is one of the green and mild methods of artificial nitrogen fixation, promising as an alternative to replace the existing industrial process. Under the requirements of green chemistry and sustainable development, the design and development of highly active and stable electrocatalysts is very important for improved synthesis performance. Mimicking from the natural nitrogenase, Fe and Mo based catalysts have attracted much attention due to their superior catalytic performance for N 2 adsorption and activation. In this work, an interfacial engineering strategy has been used to prepare a Fe, Mo-bimetallic electrocatalyst for the electrosynthesis of NH 3 . In detail, the pre-pyrolyzed biochar-based Fe 2 O 3 composites were decorated with nano-flowered MoS 2 /MoO 2 hybrids by a solvothermal process (MoS 2 /MoO 2 @Fe 2 O 3 /BC). As confirmed by the extensive characterization, the further modification not only introduced functional counterparts into the electrocatalysts but also regulated the morphology of the nanostructure. The electrochemical tests showed that the highest NH 3 yield rate of MoS 2 /MoO 2 @Fe 2 O 3 /BC was 4.87 μg h − 1 cm −2 and highest FE was 16.5% in 0.1 M Na 2 SO 4 . The catalytic stability and durability were also presented in the longtime electrolysis and cycling experiments. The improved catalytic performance of decorated catalyst, as evidenced by the comparison with Fe 2 O 3 /BC, is attributed to the increased electrocatalytic active area, the moderated hydrophilicity, and the synergistic effect of Fe, Mo-bimetallic active sites. This study provides a new perspective for the design and development of low-cost transition metal complexes as electrocatalysts for nitrogen reduction reactions.

CAS / MDL: 12054-85-2 13755-38-9
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Journal of Water Process Engineering · 2024 · IF 6.3

Enhanced uptake of antimonite onto Fe-Zr oxide-loaded MXene: Mass transfer and machine learning data mining

Fangfang Liu,Mengnan Lu,Xiao Yang,Yuedi Wang,Chunmei Wang,Xiaomin Dou

This work proposed introducing nanoscale Fe-Zr oxides onto the layered-surfaces of MXene carriers to maintain well dispersion and anchoring stabilization. The results indicated that Fe-Zr oxide/MXene has a superior adsorption capacity of 209.1 mg/g at pH 7.0. The mass transfer of antimonite onto Fe-Zr oxide/MXene was investigated by numerical solving the homogeneous surface diffusion model. The external mass transfer coefficient ( k f ) and surface diffusion coefficient ( D S ) were determined to be 6.48 × 10 −4 and 1.86 × 10 −8  cm/min, respectively, and the latter was rate-limited. The 2-D profiles of Sb(III) diffusion within the adsorbents were visualized. Data mining and knowledge discovery using machine learning models indicated that the gradient boosting regression (GBR) model successfully predicted the test datasets. The operational conditions outweigh adsorbent properties in capacity prediction, and equilibrium concentration and adsorbent dose, are the most two important features. Using the trained GBR model, the Sb(III) adsorption capacities of MXene (Ti 3 C 2 ) and Fe-Zr/MXene were well predicted. This work provides insights on understanding the mass transfer mechanisms of Sb(III) in functionalized-MXene adsorbents and employing machine learning models for tuning the treatments for better achievements.

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MICROPOROUS AND MESOPOROUS MATERIALS · 2024 · IF 4.8

Enhancement tetracycline adsorption by amino/nitro-functionalized MIL-126(Fe) adsorbent based on the ligand installation method

Mengting Xu,Zeyu Chen,Yeyang Ni,Wanyong Yang,Xihua Xu,Qing Liu,Zhaoyang Fei,Mifen Cui,Xu Qiao

MIL-126(Fe) shows great potential for aqueous phase drug adsorption due to its permanent porosity and easy modification. Herein, we utilized the ligand installation method to introduce two ligands, 2-amino terephthalic acid (NH 2 -BDC) and 2-nitro terephthalic acid (NO 2 -BDC), into MIL-126(Fe) to prepare MIL-126(Fe)-NH 2 and MIL-126(Fe)-NO 2 , respectively. Various analytical tools were used to confirm the successful installation of the 1, 4-phthalic acid (BDC) series of ligands, as well as the successful introduction of amino (-NH 2 ) and nitro (-NO 2 ) groups. The presence of both -NH 2 and -NO 2 groups improved the adsorption of TC by the adsorbent material, with -NH 2 groups having a stronger influence on the enhancement. The experimental results indicated that MIL-126(Fe)-NH 2 had the highest adsorption performance at the optimal pH of 7, achieving a static adsorption capacity of 326.5 mg/g, which was about twice the adsorption capacity of the original MIL-126(Fe). X-ray photoelectron spectroscopy (XPS) determined that the adsorption of TC by MIL-126(Fe)-NH 2 relies mainly on π-π interaction and Fe-N coordination bonds. Furthermore, the higher adsorption capacity of MIL-126(Fe)-NH 2 can be attributed to the O-H⋯N hydrogen bonds interaction between -NH 2 and the phenolic hydroxyl group (Ph-OH) in the TC molecule.

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International Journal of Environmental Research · 2024 ·Vol. 18 ·期 6 ·1-16 · IF 2.6

Efficient Degradation of Bezafibrate Using the Fe(II)/Sulfite Process: Kinetics, Mechanism and Influence on DBP Formation

Gao Yu-qiong,Ma Jia-xin,Rao Yan-yan,Chen Ju-xiang,Gao Nai-yun

Bezafibrate (BZF), an extensively used lipid-regulating agent, has been frequently detected in aqueous environments. In this work, we systematically investigated the Fe(II)/sulfite process for degrading BZF and its impact on disinfection byproducts (DBPs) during postchlorination. Degradation conditions were optimized by adjusting the pH, sulfite concentration, Fe(II), and BZF concentration. Under the conditions of pH = 4, [BZF] 0  = 5 μM, [Fe(II)] 0  = 25 μM, and [sulfite] 0  = 250 μM, the BZF removal efficiency reaches 97.9% in 15 min. Sulfate radicals (SO 4 ●– ) and singlet oxygen ( 1 O 2 ) are recognized as the main reactive agents, with Fe(IV) also contributing to the removal of BZF. Common anions (Cl − and HCO 3 − ) and humic acid generally impede the degradation process, except that trace amounts of Cl − can slightly accelerate BZF degradation. A total of ten products are recognized by ultra high performance liquid chromatography and quadrupole time-of-flight mass spectrometry, and four major degradation pathways are proposed: hydroxylation, cleavage of amino bonds, removal of fibrate chains, and dechlorination. Meanwhile, the toxicity assessment shows that the majority of products exhibit lower biological toxicity and less bioaccumulation potential than BZF itself. The Fe(II)/sulfite pretreatment alters the DBP formation potential, especially when Br − is present. The formation of trichloromethane (TCM) is diminished following pretreatment with the Fe(II)/sulfite process, whereas a noticeable increase in the formation of dichloroacetonitrile (DCAN) is found. Moreover, Fe(II)/sulfite pretreatment enhances the formation of brominated DBPs. Therefore, special consideration should be given to DBP formation when a Fe(II)/sulfite system is employed as a pretreatment for the removal of BZF in water. Graphical abstract

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