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Advanced Materials Interfaces · 2021 ·Vol. 8 ·期 21 ·2101544 · IF 6.147

Solvent-Free Mussel-Inspired Adhesive with Rapid Underwater Curing Capability

Guozheng Xia,Mei Lin,Yi Jiayu,Hu Jinkang,Li Bowen,Youbing Mu,Xiaobo Wan

How to realize fast and strong underwater adhesion has gained much attention recently. Although some mussel-inspired adhesives that can be cured underwater have been reported, reports on underwater adhesion with both high bonding strength and rapid curing capability are still rare. Furthermore, organic solvents are generally utilized in these adhesives, which are eco-unfriendly. Here, by taking advantages of the strong underwater adhesion capability of catecholic groups in mussel adhesion proteins (MAPs) and the fast curing capability of polyurethane (PU) prepolymer, a facile yet powerful strategy towards a fast-curing mussel-inspired underwater adhesive is reported. The biomimetic adhesive, PUP-PPG-DBHP, is a liquid composed of isocyanate-terminated polypropylene glycol (PPG) and isocyanate-terminated dopamine bis(hydroxymethyl)propionate (DBHP), which can be directly applied underwater without solvent dilution and reach an average bonding strength around 1.2 MPa at a curing time of only around 30 s on glass substrates. Meanwhile, underwater curing process of PUP-PPG-DBHP shows good tolerance toward pH value, ionic strength, and temperature change. Such an engineering adhesive opens an innovative and facile route to a feasible solution for underwater engineering field.

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BIOTECHNOLOGY PROGRESS · 2021 ·Vol. 38 ·期 1 ·e3218 · IF 2.681

Efficient enzymatic synthesis of L-ascorbyl palmitate using Candida antarctica lipase B-embedded metal-organic framework

Xiao-Jian Zhang,Feng-Yu Qi,Jia-Mei Qi,Fei Yang,Jiang-Wei Shen,Xue Cai,Zhi-Qiang Liu,Yu-Guo Zheng

The Candida antarctica lipase B (CALB) was embedded in the metal-organic framework, zeolitic imidazolate framework-8 (ZIF-8), and applied in the enzymatic synthesis of L -ascorbic acid palmitate (ASP) for the first time. The obtained CALB@ZIF-8 achieved the enzyme loading of 80 mg g −1 with 11.3 U g −1 (dry weight) unit activity, 59.8% activity recovery, and 92.7% immobilization yield. Under the optimal condition, ASP was synthesized with over 75.9% conversion of L -ascorbic acid in a 10-batch reaction. Continuous synthesis of ASP was subsequently performed in a packed bed bioreactor with an outstanding average space–time yield of 58.1 g L −1 h −1 , which was higher than ever reported continuous ASP biosynthesis reactions.

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JOURNAL OF ELECTRONIC MATERIALS · 2022 ·Vol. 51 ·期 3 ·1128-1136 · IF 2.047

Vapor-Phase Polymerization of PEDOT for Wearable Fabric Pressure Sensors

He Yi,Li Ying,Yuan Ying,Shu Jun,Deng Xiaoyan,Li Lu

Wearable pressure sensors with an ultra-wide linearity range and high sensitivity have atttracted increasing interest on account of their great potential applications in artificial tactile sensing, human health monitoring and care systems. Herein, poly(3,4-ethylenedioxythiophene) (PEDOT) was in situ synthesized on non-woven fabric and served as the sensing layer to realize highly reliable wearable all-fabric pressure sensors. Because of the surface microstructure of the PEDOT-coated fabric, such pressure sensors exhibited excellent performance, which included a high sensitivity of 5.95 kPa -1 , wide working range (0-200 kPa) and fast response/recovery time (11/15 ms). Their practical applications in human physiological signal monitoring are further demonstrated, showing their potential as wearable electronics in health monitoring.

CAS / MDL: 10025-77-1 288-32-4
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Highly efficient and selective H2S capture by task-specific deep eutectic solvents through chemical dual-site absorption

Mingzhen Shi,Wenjie Xiong,Xiaomin Zhang,Jialan Ji,Xingbang Hu,Zhuoheng Tu,Youting Wu

Highly efficient and selective H 2 S capture is of great scientific significance for natural gas sweetening. However, there was seldom research concerned about the chemical absorption of H 2 S in deep eutectic solvents (DESs) and the absorption capacity is hard to be satisfactory. In this work, we propose a new strategy of designing task-specific DESs endowed with chemical dual sites for H 2 S capture. Therefore, four task-specific DESs bearing with tertiary amine and acetate anion, including [C 1 -TMHDA]Ac-MDEA (1:2), [C 1 -TMHDA]Ac-Pyrol (1:2), [C 1 -TMHDA]Ac-AA (1:2), and [C 1 -TMHDA]Ac-Im (1:2), were designed and prepared. Among them, [C 1 -TMHDA]Ac-MDEA (1:2) showed the unprecedented H 2 S absorption capacity of 1.44 mol/mol at 313.2 K and 1.0 bar, surpassing all the reported absorbents. The interaction mechanism was elucidated by both spectroscopic analysis and quantum chemical calculations. In addition, five consecutive absorption–desorption cycles were performed and evaluated the recyclability of [C 1 -TMHDA]Ac-MDEA (1:2) by heating and evacuating. Compared with other absorbents, these task-specific DESs represent prominent superiority on both H 2 S absorption capacity and H 2 S/CO 2 selectivity, which are expected to be excellent alternatives in the field of acid gas separation.

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JOURNAL OF MOLECULAR LIQUIDS · 2021 · IF 6.165

Tuning the CO2 absorption and physicochemical properties of K+ chelated dual functional ionic liquids by changing the structure of primary alkanolamine ligands

Zelalem Anja Zema,Tingting Chen,Hegang Shu,Yingjie Xu

To reveal the effects of the alkyl substitutions at alpha (α) or beta (β) position adjacent to amino group of primary alkanolamine ligands on CO 2 absorption and physicochemical properties of metal chelated dual functional ionic liquids (DFILs), four DFILs were prepared by reacting potassium imidazole salt (KIm) with alkanolamine ligands, including 2-amino-2-methyl-1-propanol (AMP), 2-amino-1-butanol (AMB), DL-1-amino-2-propanol (DLAMP), and monoethanolamine (MEA). CO 2 absorption behavior and mechanism of DFILs were studied, and density ( ρ ), speed of sound ( u ), and viscosity ( η ) of DFILs were measured to correlate with the CO 2 absorption performance. DFT calculations were employed to explore the influence of the interactions between K + and alkanolamine on the CO 2 absorption and physicochemical properties of DFILs. The results show that CO 2 capacity at 333.2 K is as follows: [K(AMP) 2 ][Im] > [K(AMB) 2 ][Im] > [K(DLAMP) 2 ][Im] > [K(MEA) 2 ][Im], indicating that the introduction of alkyl group at α or β position of alkanolamines can enhance CO 2 capacity, and the effect of the α position is more significant than the β position. Both ρ and u follow the order: [K(AMP) 2 ][Im] < [K(AMB) 2 ][Im] < [K(DLAMP) 2 ][Im] < [K(MEA) 2 ][Im], while η is in the reverse order. Moreover, the saturated CO 2 capacity of DFILs has an approximately linear relation with the thermal expansion coefficient. DFT calculations show that the presence of the alkyl group at α or β position of alkanolamines reduces the Mulliken charge of N and O atom, thereby weakening the cation coordination interaction between K + with ligand, resulting in the decrease in ρ and u of DFILs. Moreover, the decrease in the Mulliken charge of N and O atom in alkanolamine leads to the increase of chelated cation-[Im] − interaction, thereby increasing η of DFILs. Consequently, [K(AMP) 2 ][Im] exhibits higher CO 2 capacity and good reversibility, due to the fact that CO 2 can react with the chelated cation and [Im] – simultaneously. The present study provides a new method for effectively regulating the performance of DFILs.

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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.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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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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Chemosensors · 2021 ·Vol. 9 ·期 8 ·236 · IF 3.398

Fabrication of an All-Solid-State Carbonate Ion-Selective Electrode with Carbon Film as Transducer and Its Preliminary Application in Deep-Sea Hydrothermal Field Exploration

Chuqing Zhang,Yang He,Jianbo Wu,Manqing Ai,Wei Cai,Ying Ye,Chunhui Tao,Pingping Zhang,Quan Jin

Real-time measurements of carbonate ion concentrations in the ocean are critical to advancing marine environmental monitoring and research into deep-sea hydrothermal activity. Herein, we report the first example of deep-sea hydrothermal field exploration using a carbonate ion-selective electrode (ISE). The novel carbonate ISE was composed of a Ni wire as substrate, carbon film as transducers and carbonate-selective membrane layers. This paper describes the preparation process of the electrode and characterises its performance via scanning electron microscopy (SEM) and electrochemical analysis. The detection limit of the electrode for CO32−is 2.821 × 10−6mol/L, the linear response range is 1.0 × 10−5–1.0 × 10−1mol/L and the Nernst slope was −30.4 mV/decade. In April 2021, the carbonate ISE was mounted on multi-parameter sensors with pH and Eh (redox) electrodes for the search of hydrothermal activity at the Southwest Indian Ridge. The simultaneous potential anomalies appeared at this carbonate electrode with the pH and Eh electrodes when passing through the hydrothermal field. The study of the hydrothermal field was supported by the in situ camera video and the sulphide samples. Additionally, the carbonate electrode provides enhanced information of water chemistry for the study of the hydrothermal field.Keywords:ion-selective electrode;carbonate determination;carbon film;hydrothermal field

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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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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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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

On the stability of imidazolium and benzimidazolium salts in phosphoric acid based fuel cell electrolytes

Hongying Tang,David Aili,Kang Geng,Jian Gao,Qingfeng Li,Nanwen Li

Polymers containing organic cations are considered as promising materials for phosphoric acid (PA) doped high temperature polymer electrolyte membranes (HT-PEMs) due to higher PA retention and wider operation temperature range. However, the thermal/acidic stability of the organic cations remains to be determined. Herein, a series of model cations based on various (benz)imidazoliums are designed and prepared to assess the stability on molecular level under simulated operating conditions for HT-PEM fuel cell. NMR analysis indicates that C2, C4 and C5 substitutions show little effect on the stability while N1 and N2 substitutions show opposite effect. Among the N -functionalized derivatives, N , N -dimethyl (benz)imidazolium cations are fully stable while N -benzyl imidazoliums degraded severely due nucleophilic substitution with H 2 PO 4 − . On this background, blend membranes based on fully methylated polybenzimidazole (PBI) are prepared, and the swelling is balanced by introducing pristine PBI. The proton conductivity of the PA doped blending membrane with IEC of 1.2 mmol g −1 reaches 165 mS cm −1 and a peak power density of 863 mW cm −2 is demonstrated in H 2 /O 2 fuel cell test. These results lay a solid foundation for designing and developing durable high-performance HT-PEMs and fuel cell devices for green energy conversion applications.

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