JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2018
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IF 2.196
Xiaofeng Li,Xiaobang Liu,Dongshun Deng
The solubility data of CO2 in four azole-based deep eutectic solvents (DESs), prepared from azoles (imidazole, Im; 1,2,4-triazole,Tri) and acetylcholine chloride (ACC), were reported at temperatures of 303.15, 313.15, 323.15, and 333.15 K under a pressure range of (20.0- 600.0) kPa using the isochoric saturation method. Henry’s constants and thermodynamic properties of standard Gibbs free energy, enthalpy, and entropy changes of CO2 dissolution were derived by correlating the data. Results demonstrated that ACC-Im DESs (Hm = 1.91–4.46 MPa·kg·mol–1) possess higher capacities of CO2 than CC-Tri ones (Hm = 2.66- 4.58 MPa·kg·mol–1). The CO2 solubility increased with rising pressure, mole ratio of Im to ACC, and decreasing temperature. All the obtained enthalpies of solution were negative. Furthermore, the comparison of dissolution capacities between present DESs and other DESs as well as some ionic liquids in the literature was conducted.
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REACTIVE & FUNCTIONAL POLYMERS
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2018
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IF 2.975
Wanbin Zhang,Guanghua Zhang,Lun Du,Ce Zhang,Lu Li,Junfeng Zhu,Jing Pei,Jiang Wu
Polybutadiene with the simultaneous presence of hydroxyl end-groups and pendant carboxyl side groups was successfully synthesized by combination of living anionic polymerization and blue light photocatalytic thiol-ene “click” reaction. Firstly, hydroxyl-terminated polybutadiene (HTPB) with high content of 1,4-butadiene unit was synthesized by living anionic polymerization using hydroxy-protected initiator, and followed by de-protection. Then, double bonds in backbone of HTPB were modified into pendant carboxyl side groups by blue light photocatalytic thiol-ene “click” reaction using Ru(bpy) 3 Cl 2 and p -toluidine as photoredox catalysts. The blue light photocatalytic thiol-ene reaction exhibit high-efficiency, and all the unsaturated bonds were modified after reacting for 5 h, in spite of that in-chain double bonds in 1,4-butadiene units are much less reactive than vinyl groups in 1,2-butadiene units. When all the double bonds were modified, the structure of resulting polymer can be deemed as carboxyl functionalized hydroxyl-terminated polyethylene . Furthermore, the solution properties of resulting polymer have been investigated by various technologies. The results showed carboxyl functionalized hydroxyl-terminated polyethylene experience a dissolution-assembly-aggregation transition process with pH value of solution decreased from 12.0 to 2.0. The mechanism of this pH-triggered phase transition behavior was supposed to depend on the ionization of carboxyl side groups at varying pH values.
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GREEN CHEMISTRY
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2018
·Vol. 20
·期 18
·4236-4244
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IF 8.586
Xiaoyan Pei,Dazhen Xiong,Yuanchao Pei,Huiyong Wang,Jianji Wang
Phase separation of microemulsions plays an important role in many applications such as oil recovery, nanomaterials synthesis, and chemical reactions. However, reversible switching from ionic liquid-based microemulsions to complete oil–water phase separation has not been reported so far. In this work, we developed a novel class of stimuli-responsive microemulsions composed of CO2-responsive ionic liquids, n-pentanol and water. The microstructures and phase behavior of the microemulsion systems before and after the bubbling of CO2 were investigated by electrical conductivity, dynamic light scattering, small-angle X-ray scattering, cryogenic transmission electron microscopy, and optical microscopy. It was found that these microemulsions could be reversibly switched from W/O monophase to complete oil–water phase separation upon alternate bubbling and removal of CO2 at atmospheric pressure. Furthermore, 13C NMR spectroscopy was used to understand the CO2-driven reversible phase separation of the microemulsions. The results suggest that the mechanism behind the reversible phase separation involved the reversible formation of bicarbonate and carbamate from the reaction between CO2 and the anions of the ionic liquids in the presence of water, which resulted in the increase of ionic strength (or vice versa) in the mixture. Using the microemulsions as microreactors, the phase separation protocol was applied in the Knoevenagel reaction for an efficient coupling of a chemical reaction, product separation, and recycling of the microemulsions.
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CELLULOSE
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2018
·Vol. 25
·期 10
·5999-6010
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IF 3.809
Ma Shanshan,Zhang Meiyun,Nie Jingyi,Yang Bin,Song Shunxi,Lu Peng
Environmental threats, especially particulate matter, toxic gases and microbial pollution, have done serious harm to human health. In this paper, biodegradable composite filters were fabricated by an in situ deposition method to isolate pollutants and inactivate bacteria. The zeolitic imidazolate framework-8@cellulose fibers (ZIF-8@CF) filters had filtration efficiency as high as 98.36% and 99.94% against 0.3 μm and 0.5 μm particles, respectively, under a pressure drop of 134 Pa. Moreover, the nitrogen adsorption capacities of the composites were about 20 times higher than those of pure cellulose filters. In addition, the Ag-based metal–organic frameworks@cellulose fibers (Ag-MOFs@CF) exhibited excellent antimicrobial activity against Escherichia coli ( E. coli ) with an inhibition zone diameter of 20.8 mm. Herein, these metal–organic frameworks@cellulose fibers (MOFs@CF) composite filters with high filtration efficiency, gas adsorption and antibacterial properties could be potentially applied in alleviating air pollution and in healthcare fields.
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CARBOHYDRATE POLYMERS
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2018
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IF 5.158
Jie Lu,Qi Kang,Jianhong Xiao,Tao Wang,Ming Fang,Li Yu
Fabrications and applications of luminescent films have been an interesting and important challenge within the realm of academia and industry. Herein, a novel fluorescence-based strategy for the H 2 O 2 detection has been developed by fabrication of stabilized, thin, transparent, and luminescent films composed of europium-containing polyoxometalates (Eu-POM) and environmentally friendly chitosan (CS) via a facile solution casting approach. In comparison with pure Eu-POM, enhanced fluorescent properties are obtained from the as-prepared Eu-POM/CS films in terms of prolonged fluorescence lifetime and a remarkable fluorescent quenching effect in the presence of hydrogen peroxide (H 2 O 2 ). The fluorescence intensity of Eu-POM/CS films exhibits a linear correlation in response to the H 2 O 2 concentration over a wide range of 1.1–66 μM, with a detection limit of 0.11 μM. Furthermore, the fluorescent films display a high detection selectivity which are capable of differentiating hydrogen peroxide (H 2 O 2 ) from the interfering species, such as sugars, l -amino acids, and other metabolites. All these advances towards the development of Eu-POM/CS films open up new applications for luminescent films, but most importantly, they can help in the far-reaching technological implementations of a simple, cost-effective method for the detection of H 2 O 2 in many fields.
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SENSORS AND ACTUATORS B-CHEMICAL
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2018
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IF 5.667
Xiaoxue Ye,Mingshi Li,Ye Hu,Zhengguo Wang,Yanying Wang,Hongping Deng,Xiaoxing Xiong,Chunya Li,Dong Sun
A photoelectrochemical immunosensor was fabricated for squamous cell carcinoma antigen (SCCA) assay with high performances by using MoSe 2 nanosheets and hollow gold nanospheres as photosensitive materials. MoSe 2 nanosheets were simply synthesized with a hydrothermal method using 1,3-di-(3-thioacetylpropyl)-imidazolium bromide (DITAPIBr) ionic liquid as a morphological controlling reagent, selenium powder, and sodium molybdate as raw materials. Hollow gold nanospheres (HGNs) were prepared by using 1,3-di-(3-bromopropyl)-imidazolium bromide ionic liquid (DIBPIBr) as functional monomer, and NaBH 4 as a reductant to interact with the HAuCl 4 solution. Subsequently, HGNs were integrated with MoSe 2 nanosheets to provide a HGNs-MoSe 2 nanocomposite. The photocurrent intensity of MoSe 2 nanosheets was significantly enhanced by the hybridization of HGNs. Furthermore, HGNs-MoSe 2 nanocomposites were coated onto a glassy carbon electrode surface to construct a platform for the immobilization of SCCA antibody (anti-SCCA), resulted in a photoelectrochemical immunosensing system for determining SCCA. Under optimized conditions, the fabricated immunosensor shows high selectivity and sensitivity towards SCCA, and exhibits a detection limit of 0.21 pg mL −1 and a linear range from 1.0 pg mL −1 to 50 ng mL −1 . Meanwhile, the practicability of the immunosensor was demonstrated by determining SCCA in clinical serum samples with high accuracy.
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MOLECULES
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2018
·Vol. 23
·期 11
·3033
·
IF 3.098
Shumei Xia,Yu Song,Xuedong Li,Hongru Li,Liang-Nian He
To circumvent the thermodynamic limitation of the synthesis of oxazolidinones starting from 2-aminoethanols and CO2and realize incorporation CO2under atmospheric pressure, a protic ionic liquid-facilitated three-component reaction of propargyl alcohols, CO2and 2-aminoethanols was developed to produce 2-oxazolidinones along with equal amount of α-hydroxyl ketones. The ionic liquid structure, reaction temperature and reaction time were in detail investigated. And 15 mol% 1,5,7-triazabicylo[4.4.0]dec-5-ene ([TBDH][TFE]) trifluoroethanol was found to be able to synergistically activate the substrate and CO2, thus catalyzing this cascade reaction under atmospheric CO2pressure. By employing this task-specific ionic liquid as sustainable catalyst, 2-aminoethanols with different substituents were successfully transformed to 2-oxazolidinones with moderate to excellent yield after 12 h at 80 °C.Keywords:ionic liquid;synergistic activation;aminoethanol;2-oxazolidinone;atmospheric CO2;sustainable catalysis
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ENERGY CONVERSION AND MANAGEMENT
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2018
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IF 6.377
Hu Pan,Hu Li,Heng Zhang,Anping Wang,Duo Jin,Song Yang
Developing an efficient one-pot catalytic process for biodiesel production from non-edible oils under mild reaction conditions remains challenging. Here, a novel process for the one-pot conversion of non-edible Firmiana platanifolia L.f. (FPLF) oil into biodiesel using inexpensive, scalable imidazolium salts-based solid acid containing both Brønsted and Lewis acid sites as the catalyst was investigated for the first time. The Brønsted-Lewis acid bifunctional catalyst ([DSI][FeCl 4 ]) was synthesized facilely and atom-economically (the final product contains the high amounts of atoms from the reactants) from 1,3-disulfonic acid imidazolium chloride ([DSI][Cl]) with FeCl 3 and was characterized by FT-IR, 1 H and 13 C NMR, N 2 adsorption–desorption, SEM-EDS, TEM, FT-IR of pyridine, NH 3 -TPD, TGA and elemental analysis. Owing to the presence of immiscible phases of oil and methanol in the reaction mixture, the effects of various co-solvents on the conversion of the FPLF oil into biodiesel were investigated, with the aim of reducing the mass transfer resistance. The results demonstrated that biomass-derived tetrahydrofuran (THF) was a superior co-solvent and could improve the reaction rate and biodiesel yield. The reaction conditions were optimized by using response surface methodology (RSM), [DSI][FeCl 4 ] exhibited excellent catalytic performance, with a high biodiesel yield of 98.7% under the following mild reaction conditions, which was superior to that of commercial resins (e.g., Amberlyst 15 and Nafion NR50). Detailed kinetic studies demonstrated that the catalytic process followed first-order kinetics and that the activation energy (83.56 kJ/mol) was relatively low compared to previous results. Thermodynamic analysis revealed that the catalytic process was non-spontaneous and that the reaction was endothermic and endergonic. Intriguingly, the catalyst was a heterogeneous catalyst during the reaction and maintained high catalytic activity after four cycles. The fuel properties of biodiesels derived from FPLF oil complied with the corresponding ASTM D6751 and EN14214 standards.
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EUROPEAN JOURNAL OF PHARMACEUTICS AND BIOPHARMACEUTICS
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2018
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IF 4.491
Huaihong Zhang,Yu Sun,Rong Huang,Hui Cang,Zhaosheng Cai,Baiwang Sun
Combination of chemotherapy with photothermal therapy (PTT) demonstrate highly desirable for efficient medical treatment of tumor. At present works, camptothecin (CPT)-containing polymeric prodrug (PCPT) were fabricated by polymerization of a pH-sensitive camptothecin (CPT) prodrug monomer and MPC using reversible addition-fragmentation transfer (RAFT) strategy. The pH-sensitive polymeric prodrug was tethered onto surface of polydopamine (PDA) nanoparticles by amidation chemistry for combination of chemotherapy with photothermal therapy. Specifically, the active CPT quickly released from the multifunctional nanoparticles in acidic microenvironment ascribe to the cleavage of bifunctional silyl ether linkage. Meanwhile, the PDA could convert the near infrared (NIR) light energy into heat with high efficiency, which makes the resulted nanoparticles an effective platform for photothermal therapy. In vitro analysis confirmed that the PDA@PCPT nanoparticles could be efficiently uptaked by HeLa cells and deliver CPT into the nuclei of cancer cells. The cell viability assays indicated an evident in vitro cytotoxicity to HeLa cancer cells under 808 nm light irradiation. Significant tumor regression was also observed in the tumor-bearing mice model with the combinational therapy provided from the PDA@PCPT nanoparticles. The PDA@PCPT multifunctional system which was achieved by a facile route should be a potential candidate in the anti-cancer field due to the synergistic therapeutic effect, which is superior to any single approach.
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International Journal of Nanomedicine
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2018
·
IF 4.37
Chen Shao,Kun Shang,Huaibao Xu,Yu Zhang,Zhichao Pei,Yuxin Pei
Background Photodynamic therapy is a safe, noninvasive modality for cancer therapy, in which the photosensitizer (PS) is a crucial component. Hypericin (Hy) is a promising PS; however, its clinical application is significantly limited by its poor hydrophilicity. Materials and methods To overcome the clinical application limitation of Hy, a novel strategy is developed here by entrapping Hy into polydopamine (PDA) film formed on the surface of magnetic iron oxide nanoparticles (MNPs) through the self-polymerization of dopamine under alkaline condition. The amount of Hy in the Hy-entrapped PDA–MNP composite nanoparticles (denoted as PHMs) was measured by spectrophotometry. Furthermore, lactose, as the targeting ligand to asialoglycoprotein receptors, was conjugated to the surface of the PHMs by taking advantage of the spontaneous reaction of PDA with amino groups. Results Spectrophotometry analysis revealed that the amount of Hy in the PHMs was 72 μmol g −1 PHMs. The fabricated Hy-entrapped glyconanoparticle (Lac-PHM) exhibited excellent water dispersibility, stability, and selectivity for asialoglycoprotein receptors overexpressing HepG2 cells. Atomic absorption spectroscopy analysis showed that the amount of the Lac-PHMs taken in HepG2 cells was 2.1-fold higher than that of the triethylene glycol-modified PHMs. The results of intracellular reactive oxygen species generation detection, cytotoxicity study, and apoptosis detection indicated that the Lac-PHMs had a satisfying photodynamic effect to HepG2 cells. Conclusion The strategy developed in this work offers great potential for delivery of a variety of hydrophobic PSs.
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Journal of the Taiwan Institute of Chemical Engineers
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2018
·
IF 3.849
Bin Jiang,Yang Chen,Luhong Zhang,Xiaowei Tantai,Haozhen Dou,Yongli Sun
In this work, a novel strategy was reported for improving SO 2 capture through multiple-site interactions of N-imidazole derivative. The tris (2-(1-H-imidazole-1-y1)ethyl) amine (TIA) was designed, synthesised and mixed with water to form the mixed absorbents for SO 2 absorption. The physical properties were determined and the mixed absorbents exhibited low densities and viscosities, which are beneficial to the mass and heat transfer. The SO 2 absorption reached equilibrium rapidly within 60 s and as high as 2.09 mol SO 2 per mol TIA could be absorbed at low SO 2 concentration (<2 kPa). With increasing the mass ratio of TIA in the aqueous absorbents to 50%, more than 6.2 mol/kg absorbent absorption performance was obtained. The desorption was carried out at 80 °C and the recycling performance was excellent without any change during 5 cycles. High SO 2 /CO 2 selectivity was achieved due to the suitable basicity of the absorbents. In addition, the absorption mechanism was established and proved by FTIR and 1 H NMR. Thermodynamic analysis was determined using gPROMS, which suggested the pK a of the TIA varied in a proper range for SO 2 capture. Overall, the novel mixed absorbents with excellent physical properties and high SO 2 absorption capacity have much potential for flue gas desulfurization.
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LANGMUIR
·
2018
·
IF 3.789
Yongxian Guo,Jie Lu,Qi Kang,Ming Fang,Li Yu
Supramolecular materials assembled by amide-functionalized surface active ionic liquid, N-dodecyl-N′-acetamido imidazolium bromide ([C12ImCONH2]Br), and europium-containing polyoxometalates (Eu-POM) were fabricated in aqueous solution by a one-step method via ionic self-assembly strategy. The [C12ImCONH2]Br/Eu-POM supramolecular structures exhibit favorable fluorescence properties and represent a 15-fold increase in quantum yield (∼13.68%) compared to Eu-POM. Besides, more fluorescence was quenched obviously with the increasing concentration of dopamine (DA) (within the range of 0–100 μM), based on which DA monitoring could be achieved. The detection limit was identified to be 0.1 μM. The supramolecular nanoparticles are highly specific for the detection of DA. In addition, the hybrid assemblies display not only low cytotoxicity but also excellent biocompatibility to MC3T3-E1 cells. As a result, as-prepared supramolecular materials with these superior properties show the promising application in some fields such as biochemistry and biomedical science.
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