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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Chemically tunable DILs: Physical properties and highly efficient capture of low-concentration SO2

Dan Li,Yong Kang,Jie Li,Zongchi Wang,Zhinan Yan,Kai Sheng

As a successive work towards exploring suitable IL-based absorbents for SO 2 absorption from flue gas, we developed a species of new dicationic ionic liquids (DILs) with the combination of ether-functionalized dication and N-heterocyclic anions. These dual-functionalized DILs possessed high thermal stability, low vapour pressure, and high SO 2 capacity. The solubilities of SO 2 in the DILs increased with declining of the temperature and elevating of the SO 2 concentration. Notably, the available loading capacity of SO 2 in DIL 4 was up to 0.267 g SO 2 ·(g DIL) -1 at 313.2 K when the concentration of SO 2 in the feed gas was 2000 ppm, which was exceedingly significant for trapping SO 2 from the flue gas with low content of SO 2 . The regeneration experiments demonstrated that the absorption capacities of SO 2 in DIL 4 kept unchanged after six successive cycles of absorption/desorption. The absorption mechanisms based on the results of 1 H NMR, FTIR analysis and quantum chemical calculations indicated that both physical and chemical interactions between the SO 2 molecules and DIL 4 could be found in spite of different concentrations of SO 2 .

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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2021 · IF 5.279

Exo III-Catalyzed Release of a Zn2+-Ligation DNAzyme to Drive the Strand Displacement Reaction and Gold Aggregation for the Homogeneous Bioassay of Kanamycin Antibiotics

Yiming Xie,Haiyan Wang,Xinyue Yuwen,Guosong Lai

Herein, we combine the exonuclease III (Exo III)-catalyzed release of a Zn2+-dependent ligation DNAzyme with the DNAzyme-driven strand displacement reaction (SDR) to develop a novel homogeneous colorimetric bioassay method for kanamycin (Kana) antibiotic detection. Upon the biorecognition reaction between Kana and a designed hairpin DNA, the DNAzyme-containing strand can be catalytically released by Exo III. Then, this DNAzyme will catalyze the ligation of two oligonucleotides to cause a SDR and the aggregation of gold nanoparticles (Au NPs) labeled by two linker DNA strands. Due to the aggregation of Au NPs for colorimetric signal transduction and the Exo III and SDR-assisted dual signal amplification, this method shows a wide linear range of 5 orders of magnitude and a very low detection limit down to 8.1 fg mL–1. Together with its excellent selectivity, repeatability, reliability, and convenient manipulation, the proposed method shows a great potential for the food quality monitoring application.

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ACS Applied Polymer Materials · 2021 · IF 4.089

Design, Synthesis, and Adhesion of Fluorescent Conjugated Polymers with Pendant Catechol Groups

Hao Zhan,Jiajun Chen,Chi Zhang,Jincheng Zhang,Li-Juan Fan

Incorporating conjugated polymers with functionalities to provide good adhesion to solid substrates is favorable to prepare fluorescent solid materials for various applications. Inspired by the wide range and robust adhesion property of mussel, a series of conjugated polymers with the poly[p-(phenylene ethynylene)-alt-(thienylene ethynylene)] backbone and pendant catechol groups via Sonogashira coupling polymerization were designed and synthesized. The contents of catechol groups were precisely tuned through copolymerization, followed by selective deprotection. For comparison, similar polymers with pendant phenol groups were also synthesized. The conjugated polymers were demonstrated to have expected chemical structures via systematic characterizations. All the polymers had good solubility in common organic solvents and displayed strong fluorescence in solution. To evaluate the adhesion performance of different polymers, fluorescent silica microspheres were selected as the substrate for loading the abovementioned polymers via immersing the silica microspheres into solutions of conjugated polymers. To find out the loading amount, a calibration curve for each polymer was set up based on the linear relationship between the fluorescence intensities of the suspension of microspheres and the polymer concentrations. The loading amounts of catechol-functionalized polymers were significantly higher than those of phenol-functionalized polymers; the highest loading amount is over 14-fold of the amount of the control polymer without any catechol/phenol functionality. By combining the abovementioned results with the preliminary mechanism investigation based on the solvent washing, it was concluded that catechol functionality and its content in the polymers greatly affected the adhesion performance. The multidentate interaction provided by catechol groups may enable the conjugated polymers to be widely used for fluorescence coating and staining of a variety of substrates.

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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Superhigh and reversible NH3 uptake of cobaltous thiocyanate functionalized porous poly ionic liquids through competitive and cooperative interactions

Li Luo,Jiaran Li,Xiaoyan Chen,Xuegong Cao,Yibang Liu,Zhixin Wu,Xiaoyan Luo,Congmin Wang

In this work, porous PIL-TAs were reported for superhigh capacity and reversible NH 3 uptake, where PIL-TAs are cobaltous thiocyanate (Co(II)(SCN) 4 2- , TA) functionalized poly ionic liquids (PILs). Due to the structural support of TA as well as the interactions between TA and imidazolium cation, the PIL-TAs possess porous structure and optimized properties. Superhigh NH 3 uptake capacity of 13.2–20.1 mmol g −1 at STP of PIL-TAs was achieved, which is higher than most of the reported sorbents. In detail, the cooperative interactions including the NH 3 coordinating with Co(II) instead of SCN - and hydrogen bonding of C2H in imidazolium (C2H…NH 3 ) benefit to high capacity of NH 3 uptake. Reversely, the NH 3 release would be directed by the competition of the free SCN - with NH 3 to reform PIL-TAs. The competitive interaction with SCN - promotes NH 3 release by temperature and pressure swinging, which contributes the adsorbents recyclable. The cooperative and competitive interactions make these PIL-TAs possess high gas capacity and feasible desorption, which might be a potential strategy for designing novel gas sorbents.

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Nanoscale · 2021 ·Vol. 13 ·期 38 ·16197-16206 · IF 7.79

Gadolinium–porphyrin based polymer nanotheranostics for fluorescence/magnetic resonance imaging guided photodynamic therapy

Wandi Chen,Junkai Zhao,Mengfei Hou,Mo Yang,Changqing Yi

Nanotheranostics for fluorescence/magnetic resonance (FL/MR) dual-modal imaging guided photodynamic therapy (PDT) are highly desirable in precision and personalized medicine. In this study, a facile non-covalent electrostatic interaction induced self-assembly strategy is developed to effectively encapsulate gadolinium porphyrin (Gd-TCPP) into homogeneous supramolecular nanoparticles (referred to as Gd-PNPs). Gd-PNPs exhibit the following advantages: (1) excellent FL imaging property, high longitudinal relaxivity (16.157 mM−1 s−1), and good singlet oxygen (1O2) production property; (2) excellent long-term colloidal stability, dispersity and biocompatibility; and (3) enhanced in vivo FL/MR imaging guided tumor growth inhibition efficiency for CT 26 tumor-bearing mice. This study provides a new strategy to design and synthesize metalloporphyrin-based nanotheranostics for imaging-guided cancer therapy with enhanced theranostic properties.

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2021 · IF 4.539

A sensitive chemosensor for nitro-containing compounds based on Au nanoclusters/Ba2+ co-assembly system: The crucial role of ligands to metal charge transfer

Jinglin Shen,Yue Bi,Hao Zhang,Liandi Xu,Jin Feng,Wei Qi

Gold nanoclusters (AuNCs) are a class of promising inorganic-organic hybrid nanomaterials with exceptional photoluminescent properties. The understanding of their photoluminescent mechanism is important for developing functional AuNCs-based materials. In this work, thiobarbituric acid-modified AuNCs (TBA-AuNCs) was prepared and its photoluminescent property was modulated through co-assembly with Ba 2+ . The emission intensity was sharply enhanced with the formation of TBA-AuNCs/Ba 2+ complex. Structural characterization including transmission electron microscopy , scanning electron microscopy and X-ray photoelectron spectroscopy confirmed the hybridization of TBA-AuNCs with Ba 2+ . The pH-dependent photoluminescence as well as zeta potential measurements demonstrated that the ligand to metal charge transfer (LMCT) is crucial for the regulation of emission property of the TBA-AuNCs/Ba 2+ . Based on this special photoluminescent mechanism, the TBA-AuNCs/Ba 2+ complex was employed as a chemical sensor for nitro-substituted aromatic compounds . The emission intensity of TBA-AuNCs/Ba 2+ selectively displayed sharp quenching in response to 2-methyl-4-nitroimidazole among various imidazole derivatives. Simultaneously, the complex also showed high sensitivity toward p -nitroaniline and 2-nitrophenol. Therefore, the developed TBA-AuNCs/Ba 2+ assemblies are potential in detecting the nitro-containing compounds, which will find applications in pharmaceutical analysis, environmental protection and other related fields.

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ACS Applied Energy Materials · 2021 · IF 6.024

Efficient Solid-State Electrolytes Based on Aryl-Modified Imidazolium Ionic Crystals for Quantum Dot-Sensitized Solar Cells

Guojiao Zhao,Yefeng Wang,Jing-Hui Zeng,Zhaofu Fei,Paul J. Dyson

Cost-effective solid-state electrolytes with improved conductivity and device performances have received much research interest in (photo)electrochemical cells, including solar cells, secondary batteries, and so on. In this work, a series of organic ionic crystals (OICs) containing imidazolium salts modified with bulky fluorenyl and diphenylmethyl substituents and BF4 anions were synthesized and applied into quantum dot-sensitized solar cells (QDSSCs) as the matrix of solid-state electrolytes. The performance of QDSSCs employing these new OICs was evaluated by electrochemical impedance spectroscopy, Tafel plots, and incident monochromatic photon–electron conversion efficiency traces. A champion device applying imidazolium salts with nonplanar diphenylmethyl substituents and BF4 anions afforded a highest power conversion efficiency of 5.69% under AM 1.5 (100 mW·cm–2) irradiation.

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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2021 · IF 4.098

Large-scale sensitivity adjustment for Gd-HMME room temperature phosphorescence oxygen sensing

Honglin Zhang,Ting Liu,Qiuhe Li,Xiyu Zhang,Hua Zhao,Yangdong Zheng,Feng Qin,Zhiguo Zhang,Tianqi Sheng,Ye Tian

The oxygen sensing enhancement based on room temperature phosphorescence (RTP) of Gd-HMME adjusted by imidazole was studied. The phosphorescence intensity I P0 and the Stern-Volmer equations under different imidazole concentration were obtained, and the physical mechanism of imidazole regulating the oxygen quenching constant K SV was analyzed. It was found that the K SV value increased by ∼46 folds in the range of 12.4(1)–576.1(5) kPa −1 , and the large-scale variation of K SV is conducive to the realization of high precision oxygen concentration measurement in a wide range. In addition, the standard deviation σ of continuous measurement results was given, and the limit of detection (LOD) was determined to be 6.6 ppm.

CAS / MDL: 10138-52-0 288-32-4
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POLYMER TESTING · 2021 · IF 4.282

Study on the preparation and performance comparison of side-chain hydroxyl-terminated polybutadiene derivatives with narrowly molecular weight distribution used for polyurethane

Lingxiao Ma,Xiuzhong Zhu,Wanbin Zhang,Haitao Zhang,Jianyong Wang,Jianbo Qu

Hydroxy-terminated oligomers with narrow molecular weight distribution using as soft segment of polyurethane can significantly increase the modulus, tensile strength, and elongation at break of the polyurethane. Thus, design and synthesis of new hydroxy-terminated oligomers having narrow molecular weight distribution can improve the properties of polyurethane and further expand the use range of polyurethane. A set of side-chain hydroxyl-terminated polybutadiene (HTPB) derivatives were successfully synthesized by anionic polymerization and blue light photocatalytic thiol-ene reaction. Firstly, HTPB with narrow molecular weight distribution was synthesized via anionic polymerization using mono-lithium based initiator and followed by de-protection. Then, HTPB derivatives with different side-chains such as butyl, ethyl acetate, or myristyl, namely HTPB but , HTPB eac and HTPB tet , were obtained by blue light photocatalytic thiol-ene reaction using Ru(bpy) 3 Cl 2 as photoredox catalyst and HTPB as matrix polymer. Similar with HTPB, those HTPB derivatives also have narrow molecular weight distribution. Polyurethane elastomers (PUs) were synthesized with HTPB or HTPB derivatives as soft segment, toluene diisocynate (TDI) as hard segment, and 1, 4-butanediol as chain extender. Compared study the performances of polymers, the results showed that glass transition temperature ( T g ) and viscosity of HTPB derivatives were increased when short-chain side groups were introduced. But instead, T g and viscosity of HTPB derivatives was reduced following long-chain side groups being grafted. Through comparing research of properties for PUs, tensile strength is reduced and elongation at break is augmented, when side groups were introduced in HTPB backbone. Research on the contact angle tests of PUs indicated that the contact angle of PUs using HTPB, HTPB but or HTPB eac as soft segment, is similar, and PUs using HTPB tet as soft segment has a larger contact angle about 137.2 °C.

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JOURNAL OF MATERIALS SCIENCE · 2021 ·Vol. 56 ·期 34 ·19283-19295 · IF 4.22

Biocompatible mesoporous polymeric ionic liquid with high adsorption capacity for selective isolation of ovalbumin

Qi Shoujing,Zhang Chunyu,Hu Zhengjie,Chen Xuwei

Ionic liquids are becoming widely applied in the extraction/separation of biological molecules. In this study, the solidification of ionic liquid 1-hydroxyethyl-3-vinylimidazole chloride ([HVIM]Cl) was achieved via one-pot free radical copolymerisation with divinylbenzene (DVB) as a cross-linking reagent, giving a mesoporous hydrophilic polymeric ionic liquid (PIL). Mesoporous PIL possesses a large surface area of 328.32 m 2 ·g −1 and a high pore volume of 0.45 cm 3 ·g −1 . Owing to hydrophilic interactions and π–π stacking interactions, the PIL adsorbs ovalbumin (Ova) selectively with a theoretical maximum adsorption capacity of 2468.0 mg·g −1 , and this Ova adsorption fit the Langmuir model well. The captured Ova was efficiently recovered using sodium dodecyl sulphate (0.4%, m·v −1 ) with an elution efficiency of 94.7%. Circular dichroism spectra indicated that the adsorption-elution process caused no conformational changes in Ova, indicating that the prepared PIL is highly biocompatible. The practicability of this mesoporous PIL was well demonstrated by the selective adsorption of Ova from protein mixtures and the efficient isolation of Ova from chicken egg white. Graphical abstract

CAS / MDL: 78-67-1 288-32-4 77-86-1
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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 43 ·期 39 ·15700-15705 · IF 3.069

Condensation of 9-fluorenone and phenol using an ionic liquid and a mercapto compound synergistic catalyst

Yan Lei,Limei Yu,Maochang Shen,Shikang Luo,Zhanxian Gao

A series of ionic liquids (ILs) were synthesized and their Hammett acidities (H0) were determined using 4-nitroaniline as the indicator. The relationship among IL's structure, the acid strength, and the catalytic performance in the condensation reaction of 9-fluorenone with phenol was discussed. The effective H0 range of ionic liquids that can catalyse the condensation reaction was obtained. Moreover, the catalysis of the mercapto compound co-catalyst was also systematically studied. According to the analysis of how the structure of the sulfydryl co-catalyst affects the percent conversion of 9-fluorenone and the selectivity of BHPF, a mechanism for the reaction in the IL–thiol cooperative catalytic system was proposed. The present work gave a clear clue to design novel IL catalysts for the synthesis of BHPF.

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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

An artificial organic-inorganic Z-scheme photocatalyst WO3@Cu@PDI supramolecular with excellent visible light absorption and photocatalytic activity

Wengao Zeng,Tao Cai,Yutang Liu,Longlu Wang,Wanyue Dong,Hui Chen,Xinnian Xia

Tungsten trioxide (WO 3 ) has a wide application in environmental remediation due to its stability. Yet, the application of WO 3 is severely limited by its wide band gap and weak electron reduction ability. In this work, we intend to enhance the visible light absorption and photocatalytic performance by constructing an organic-inorganic Z-scheme system WO 3 @Cu@PDI. Apparently, WO 3 @Cu@PDI has excellent visible light absorption and photocatalytic degradation ability in the degradation of tetracycline hydrochloride (TC). Under visible light irradiation, the degradation rate of composites is 40 times faster than that of sole WO 3 and 5 times than PDI. The photocatalytic activity of WO 3 @Cu@PDI toward TC still kept 85% after three reuses. We revealed that this high photoactivity arisen from the efficient carriers separation and the formation of Z-scheme junction. Importantly, this Z-scheme electron transfer pathway was confirmed by thorough experimental study. This work demonstrated the significant potential of WO 3 -based inorganic-organic Z-scheme photocatalyst in environmental remediation.

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