APPLIED ORGANOMETALLIC CHEMISTRY
·
2019
·Vol. 33
·期 10
·e5145
·
IF 3.259
Zhiguo Lv,Shuying Zhang,Zhenmei Guo,Xi Cheng,Jiaomei Wang,Chao Zhang
The synthesis of alcohol ester 12 is one of the valuable industrial processes, but it was impeded by poor separating property and recycling ability of the catalytic systems. Herein, four novel DBU-based basic ionic liquids (DBILs) of [BDBU]IM, [BDBU]OH, [ODBU]IM, [[ODBU]OH were synthesized successfully by introducing the alkyl chains of 1-bromobutane or 1-bromooctane to 1,8-diazabicyclo [5.4.0] undec-7-ene (DBU), and then, employing imidazole (IM − ) or hydroxide (OH − ) as counter ions. The above obtained four ionic liquids were applied in the synthesis of alcohol ester 12 in isobutyraldehyde (IBD)/aqueous media for the first time. Interestingly, after reaction, production of alcohol ester 12 can be self-separated from ionic liquids/water (ILs/W) catalytic system automatically. Furthermore, the self-separated ILs/W can be recycled and used in next catalytic reaction for at least 5 times without obvious loss of catalytic performance. In this work, the structure, purity, thermal stability and alkalinity of DBILs were characterized systematically. [BDBU]IM shows high alkalinity and thus enhances yield of 66.17%. From thermo gravimetric analyzer (TGA), [BDBU]IM also exhibits excellent thermal stability. So [BDBU]IM was chosen for the further studying. Furthermore, quantum chemistry is applied to calculate the interaction forces and electron energies of reactants by DFT, and the calculation results illustrate the feasibility of synthetic process of DBILs. The self-separation strategy of DBILS in this work may open up a new avenue for the clean synthesis of other industrial products.
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CRYSTENGCOMM
·
2017
·Vol. 19
·期 44
·6644-6650
·
IF 3.474
Ying-Jie Jia,Yi-Gang Chen,Xiao-Ni Yao,Xian-Ming Zhang
A series of alkali earth cadmium selenites including MgCd3(SeO3)4 (1), Ca0.7Cd2.3(SeO3)3 (2), SrCd(SeO3)2 (3) and BaCd(SeO3)2 (4) are synthesized by hydrothermal reaction and studied in detail by single crystal and powdered X-ray diffractions, thermal analyses, IR and UV spectral measurements and dipole moment calculation. 1 features a 3D anionic [Cd3(SeO3)4]2− framework constructed from isolated SeO3 trigonal pyramids and 2D [Cd3O12]n layers, in which the [Cd3O12]n layer is composed of edge-shared [Cd2O10]16− dimers and butterfly-like [Cd4O20]32− tetramers. 2 shows a smooth 2D [Cd2(SeO3)3]n layer composed of unique [Cd(SeO3)]n double chains. 3 exhibits a wavelike 2D [Cd(SeO3)2]n layer constructed from corner-shared CdO6 octahedra and isolated SeO3 trigonal pyramids. 4 displays a windmill-like 1D [Cd(SeO3)2]n chain built from zigzag [CdO4]n chain motifs and isolated SeO3 trigonal pyramids. The alkali earth oxide motifs demonstrate interesting and regular changes from isolated MgO6 octahedra, CaO7 polyhedra, and SrO9 tri-capped trigonal prisms based on a ribbon chain to BaO12 icosahedra based on a brucite-like layer, and meanwhile the SeO3 groups are observed from variable tetradentate to hexadentate coordination modes. These flexible motifs reveal that cadmium selenites are strongly affected by the size of the alkali earth cations, providing a feasible approach to modulating their space structure via selection of template cation.
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MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Jun Gao,Danyang Fan,Qinghua Chu,Haixia Lyu,Zenghong Xie
In this study, a novel surface molecularly imprinted polymer (MIP) based on zeolitic imidazolate framework (MIP@ZIF-7) was prepared using dibutyl phthalate (DBP) as template via “one-pot” method, which was used for extraction and determination four phthalates (PAEs) in food samples coupled with high performance liquid chromatography (HPLC). The obtained MIP@ZIF-7 was characterized by fourier transform infrared spectrometer (FT-IR), energy dispersive spectrum (EDS), scanning electron microscopy (SEM), nitrogen adsorption–desorption and contact angle tester. The adsorption performance of the prepared ZIF-7, MIP and MIP@ZIF-7 was compared and the results showed that MIP@ZIF-7 exhibited higher adsorption capacity and selectivity for PAEs owing to combining the high specific surface area and excellent stability of ZIF and the specific recognition of MIP. Subsequently, several requisite synthesis and extraction parameters were investigated. Under the optimal conditions, the linear range of the method was 1–100 μg L −1 and the detection limits were in a range of 0.1–0.8 μg L −1 . The spiked recovery rate of PAEs from drinking water, carbonated beverages and fruit juices ranged from 77.1 ± 1.5% to 100.7 ± 3.4%, with relative standard deviation of 1.65–4.87% (n = 3). The results indicated that MIP@ZIF-7 could be effectively employed for extraction and determination trace PAEs in food.
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EUROPEAN POLYMER JOURNAL
·
2021
·
IF 4.598
Yang Chen,Jie Zhang,Wenhao Xiao,Anfu Chen,Zhixian Dong,Jinbao Xu,Wenhua Xu,Caihong Lei
1,8-Diazabicyclo[5.4.0]undec-7-ene (DBU) was used as organocatalyst to reinvestigate the ring-opening polymerization (ROP) of ε -caprolactone (CL) with benzyl alcohol (BnOH) initiator in bulk at 90 °C considering the unsuccessful ROP of CL at RT in previously reported publications. Kinetic study indicates that the PCLs could be well-designed with a controlled/living character of polymerization. The use of functional initiators, such as 2-hydroxyethyl methacrylate (HEMA), propargyl alcohol (PGA), 6-azido-1-hexanol (AHA) and methoxy poly(ethylene glycol) (mPEG) leads to end-functionalized PCLs. Accordingly, the block copolymerization of CL with δ-valerolactone (VL), trimethylene carbonate (TMC) and lactide (LA) successfully proceeded to give PCL- b -PVL, PCL- b -PTMC and PCL- b -PLA copolymers. Finally, the reaction mechanism was studied with DFT calculations and NMR measurements.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yeqiang Lu,Shiyang Li,Fuyou Chen,Hui Ma,Congjie Gao,Lixin Xue
Development of efficient absorbent materials for oil spillage clean-up and environmental pollution remediation is highly desired but remains a challenge. In this work, superhydrophobic/superoleophilic polysulfone based ZIF-7 composite (SPZ) foams were fabricated via chemical modification of polysulfone and integrating with hydrophobic coin-shaped ZIF-7 particles. The synergistic approaches provided the SPZ foams with high porosity, low density and superhydrophobic/superoleophilic features ( θ water =162.3°, θ oil =0°) and outstanding self-cleaning property. The as-prepared SPZ foams exhibited highly selective absorption capacity (up to 3800 wt%) for various kinds of oils and organic solvents. Furthermore, the SPZ foams still maintained 95.2% of its pristine absorption capacity and the θ water remained at 143.6° after ten absorption/distillation cycles. The SPZ foam showed outstanding separation ability towards different types of emulsions with separation efficiency all above 97%. The high oil/water separation efficiency and robust reusability made the SPZ foams promising absorbent in dealing with practical oil spills.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2021
·Vol. 104
·期 7
·3365-3375
·
IF 3.784
Jindi Wang,Shuai Huang,Yu Yan,Mengmeng Shang
In this work, using Ca 10.5 (PO 4 ) 7 as the structural model, a number of Eu 3+ -doped [Ca 9 Na 3x Y 1-x (PO 4 ) 7 (CNYP-I, 0 ≤ x ≤ 1/2) ← Ca 10.5 (PO 4 ) 7 → Ca 9+y Na 3/2-y/2 Y (1-y)/2 (PO 4 ) 7 (CNYP-II, 0 ≤ y ≤ 1)] phosphors were designed and synthesized through the heterovalent substitution of Y 3+ and Na + to Ca 2+ . The substitution mechanism, composition structure, luminescence performance, and thermal stability of Eu 3+ -doped CNYP-I (0 ≤ x ≤ 1/2) as well as the solid solutions of CNYP-II (0 ≤ y ≤ 1), were discussed in detail. The morphology and element composition of CNYP-I (0 ≤ x ≤ 1/2) and CNYP-II (0 ≤ y ≤ 1) solid solutions were analyzed by SEM and EDS. The PL spectra of the specimens were containing the predominant red peak of emission at 612 nm caused via the transition of 5 D 0 - 7 F 2 , indicating that Eu 3+ occupies the low-symmetry center. Moreover, the site symmetry Eu 3+ occupied changed with the x/y value. The luminous intensity of Eu 3+ -doped CNYP-I (0 ≤ x ≤ 1/2) and CNYP-II (0 ≤ y ≤ 1) phosphors at 150°C maintained about 60% of room temperature. The representative compound CNYP-I (x = 1/3) was used as the red phosphor to prepare a near-UV based white LEDs along with Ra of 80.9 and CCT of 4100 K.
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SOLID STATE SCIENCES
·
2021
·
IF 3.059
Yong Cao,Kangping Cui,Yihan Chen,Minshu Cui,Guanghong Li,Dong Li,Xiaojun Yang
Iron Oxychloride (FeOCl) was prepared by partial thermal decomposition and was studied as a heterogeneous Fenton catalyst to degrade tetracycline (TC). SEM, XRD , XPS technology were used to characterize its performance. The influencing factors of TC degradation efficiency were studied, including pH value, H 2 O 2 content, catalyst dosage and initial TC concentration. The results showed that under the optimal conditions, the degradation rate of 60 mg L −1 TC reached 92.9% within 60 min of reaction. The degradation process follows a second-order kinetic equation. Compared with other iron-based catalysts, FeOCl exhibited better catalytic and degradation effects. Moreover, FeOCl/H 2 O 2 system exhibited a wide pH range (from 3.0 to 7.0) for efficient degradation of TC and showed excellent stability and reusability. Meanwhile, based on the intermediates identified by HPLC-MS, two possible pathways for the degradation of TC were proposed. Further, the results of electron spin-resonance spectroscopy and radical quenching tests suggested that the ·OH formed in the FeOCl/H 2 O 2 system was mainly responsible for the degradation of TC.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2020
·
IF 5.647
Lei Jia,Wei Liu,Jilin Cao,Zhaoliang Wu,Chunyan Yang
In this study, multi-walled carbon nanotubes (MWCNTs) had been used to strengthen the removal of acid orange 7 (AO7) from the dyestuff wastewater by using foam fractionation. First, the surface modification of MWCNTs was performed by introducing hypochlorite groups (-OCl). The modified MWCNTs were characterized by using SEM , XRD , FTIR and Raman spectroscopy . Subsequently, the potential of modified MWCNTs as a novel collector for AO7 adsorption was examined. The adsorption conditions of modified MWCNTs towards AO7 were optimized by using response surface methodology (RSM) with a central composite design (CCD). The adsorption capacity of modified MWCNTs towards AO7 could reach 47.72 ± 0.79 mg·g −1 under the optimum conditions. The kinetics and the equilibrium adsorption data were analyzed by using different kinetic and isotherm models. According to the regression results, adsorption kinetics data were well described by pseudo-second order model, whereas adsorption isotherm data were best represented by Langmuir isotherm model. Finally, foam fractionation was performed with a batch mode. Under the suitable conditions of loading liquid volume 300 mL, modified MWCNTs dosage 180 mg, cetyltrimethylammonium bromide (CTAB) concentration 50 mg·L −1 , AO7 concentration 30 mg·L −1 , pore diameter of gas distributor 0.125 mm and air flow rate 100 mL·min −1 , the removal percentage and enrichment ratio of AO7 were 91.23% and 6.17, respectively. The decolourization ratio of solution after foam fractionation was found to be 98.66%.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2020
·
IF 3.232
Selvaraj Muthusamy,Kanagaraj Rajalakshmi,Qingxiang Xu,Yan Chen,Long Zhao,Weihua Zhu
Detection of H 2 S to analyze some diseases in living lives demands fast response, high selectivity and biocompatibility. Here we designed an azide containing coumarin attached with 8-aminoquinoline via amide backbone (ACAQ) fluorophore as the H 2 S sensing probe. Excellent response time of 6 min, high sensitivity with the limit of detection (LOD) of 14.6 nM and high selectivity with other possible interferences are revealed for ACAQ after characterized by spectroscopy, 1 H NMR titration and LC–MS measurements. The sensing strategy is explained by amide-iminol tautomerism and azide reduction. In addition, the successful visualization measurement suggests the practicability of the probe ACAQ for H 2 S detection in live samples.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2019
·
IF 2.298
Yuli Shi,Haojian Zhang,Xiaomin Hong,Xiaodong Wang
Four solvents (ethanol, isopropanol, ethylene glycol (EG), and N,N-dimethylformamide (DMF)) that can be mixed with water in any ratio were selected to determine the dissolution performance of 7-amino-4-methylcoumarin by the classical shake-flask method. The measured temperature range began at 278.15 K and ended at 303.15 K, and the pressure environment was controlled at standard atmospheric pressure (101.1 kPa). Results reveal that with the addition of organic solvents, the solubilization effect of 7-amino-4-methylcoumarin was very significant and the larger the amount of addition, the more obvious was the effect of solubilization. Not only that, the temperature change had a non-negligible effect on the dispersion of 7-amino-4-methylcoumarin; the temperature increased monotonically, and the better was the dissolution. When the external conditions were kept constant, the addition of DMF made the solubilization effect of 7-amino-4-methylcoumarin most obvious among all organic solvents used. This study involved three models, including the Jouyban–Acree model and its two variants (van’t Hoff–Jouyban–Acree model and Apelblat–Jouyban–Acree model), which were used to correlate the solubility data of 7-amino-4-methylcoumarin in aqueous cosolvent mixtures. The relative average deviation (RAD) and root-mean-square deviation (RMSD) reaches to 3.47 × 10–2 and 1.79 × 10–3 rooting in the van’t Hoff–Jouyban–Acree model. The relevant parameters obtained through model calculation and experimental means are essential for product synthesis, separation, and purification processes.
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Oxidative Medicine and Cellular Longevity
·
2019
·
IF 4.868
Lifang Sun,Min Zhu,Wei Feng,Yiping Lin,Jia Yin,Juan Jin,Yunguang Wang
Idiopathic pulmonary fibrosis (IPF) is a prototype of chronic, progressive, and fibrotic lung disease with high morbidity and high mortality. Menstrual blood-derived stem cells (MenSCs) have proven to be an attractive tool for the treatment of acute lung injury and fibrosis-related diseases through immunosuppression and antifibrosis. However, whether MenSC-derived exosomes have the similar function on pulmonary fibrosis remains unclear. In the present study, exosomes secreted from MenSCs (MenSCs-Exo) were verified by transmission electron microscope (TEM), nanoparticle tracking analyzer (NTA), and western blotting. And MenSC-Exo addition significantly improved BLM-induced lung fibrosis and alveolar epithelial cell damage in mice, mainly reflected in BLM-mediated enhancement of the fibrosis score, blue collagen deposition, dry/wet gravity ratio, hydroxyproline and malondialdehyde levels, and downregulation of glutathione peroxidase, which were all robustly reversed by MenSC-Exo management. Additionally, BLM- and TGF-β1-evoked cellular reactive oxygen species (ROS), mitochondrial DNA (mtDNA) damage, and cell apoptosis were rescued by MenSCs-Exo in vivo and in vitro. Further study indicated that the MenSCs-Exo could transport miRNA Let-7 into recipient alveolar epithelial cells. Let-7 inhibitor administration significantly blocked the exosome-mediated improvement role on lung fibrosis in mice. Mechanistically, Let-7 was able to regulate the expression of lectin-like oxidized low-density lipoprotein receptor-1 (LOX1) through binding to its 3-UTR region. Forced expression of LOX1 promoted the expression of apoptosis-related protein and mtDNA damage markers via regulating NLRP3 which was also confirmed in BLM model mice under the combination therapy of the exosome and Let-7 inhibitor. Collectively, this study demonstrates that exosomal Let-7 from MenSCs remits pulmonary fibrosis through regulating ROS, mtDNA damage, and NLRP3 inflammasome activation. This provides a new approach of exocytosis on the treatment of fibrotic lung disease.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Qi Yang,Han Yeong Kaw,Jing Yu,Xuejing Ma,Kun Yang,Lizhong Zhu,Wei Wang
The extensive prescription of fluoroquinolone antibiotics has resulted in their ubiquitous presence in the environment, fueling the ongoing development of antibiotic resistance. Besides antibiotics, fluoroquinolone production intermediates, an overlooked category of pollutants that oftentimes possess the intact fluoroquinolone core structure, may also contribute to this public health crisis. To assess their relative potency and collectively examine the structural effects of fluoroquinolones on resistance development, wild-type Escherichia coli K12 was exposed to ten fluoroquinolone antibiotics and five intermediates at their environmentally relevant concentrations for 30 days. Phenotypic resistance alterations revealed that the absence of the C7 ring system in fluoroquinolones significantly impaired their capacity to induce resistance in E. coli, potentially due to diminished oxidative DNA damage and gyrase-mediated dsDNA breaks. Genetic and transcriptional analyses indicated that a uniform resistance mechanism emerged under both antibiotic and intermediate stress. Quantitative structure–activity relationship (QSAR) analysis further emphasized the positive impact of both basic nitrogenous heterocyclic rings at C7 (particularly the hydrogen-bond-donor pharmacophores) and aromatic rings at N1 in promoting resistance development, while highlighting the adverse effects of hydrophobic and hydrogen-bond-donor groups at N1. A robust QSAR model was developed and applied to assess the relative risks of other 105 fluoroquinolones. This study underscored the direct role of fluoroquinolone production intermediates in promoting environmental antibiotic resistance and illustrated how different structural features of fluoroquinolone pollutants will influence this process, offering theoretical insights for future antibiotic design and environmental regulation efforts.
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