ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Yunlong Yang,Yuanlong Guo,Jili Yuan,Haibo Xie,Chengtao Gao,Tianxiang Zhao,Qiang Zheng
The design and facile preparation of ionic liquids (ILs)-functionalized polymer materials is a hot research topic due to their potential wide applications. Herein, taking the reaction advantage of a cyclic anhydride with an alcoholic compound to atom-economically generate a carboxyl ester pending a carboxylic acid moiety, porous organic framework (POF) materials pending carboxylic acids and imidazolium-based ILs (CILs-POFm) were facile synthesized via the acylation reaction of hydroxyl group-functionalized ILs with a styrene maleic anhydride copolymer. The CILs-POFm material properties were facilely adjusted by changing the molar ratio of the mono-hydroxyl-functionalized ILs to the dihydroxyl-functionalized ILs. CILs-POFm materials showed abundant mesoporous structures with a porous diameter of approximately 23.83–48.16 nm, a surface area of up to 274.4 m2 g–1, and a superior CO2 adsorption capacity of 1.71–2.14 mmol g–1 at 273 K and 1 atm. As a proof of concept application, the coupling reaction of epoxides with CO2 to produce cyclic carbonates was studied by using the CILs-POFm materials as catalysts under solvent-free and co-catalyst-free conditions. The findings indicated that the CILs-POF0.5 exhibited a satisfactory catalytic activity and reusability for a large scope of epoxides. Based on the experimental results and density functional theory (DFT) simulations, a synergetic catalytic mechanism was proposed based on the pended carboxylic acidic groups and IL groups. This study not only provided an atom-economic strategy to prepare POFs pending both carboxylic acids and ILs, but also showed new insights into the design of functionalized POF materials with great application potential in energy storage materials, separation, and green catalysis.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Wentao Zheng,Guibing Xia,Guangwen Yu,Qian Cai,Xiankun Wu,Weizhong Shi
A series of low viscous deep eutectic solvents composed of 1,8-Diazabicyclo[5.4.0]undec-7-ene (DBU) and N-heterocyclic compounds were designed and synthesized as NO trapping agents. These DESs exhibited low viscosity of 10.02 mPa·s and excellent NO absorption capacity up to ∼ 5.10 mol·kg −1 at 293.2 K and atmospheric pressure. The N-heterocyclic compounds were found to play a dominant role in the absorption, and the absorption behavior could thus be adjusted by the molar ratio of DBU to N-heterocyclic compounds. With the assumption of complex formation between NO and DESs, the reaction equilibrium thermodynamic model (RETM) was developed to correlate the experimental solubilities of NO. The thermodynamic parameters, such as the equilibrium constant K , the Henry’s constant H and the enthalpy change Δ H , were thus calculated to evaluate the absorption process. In addition, through a combination of the experimental absorption capacities, the RETM modeling results and the spectroscopic investigations, it was proposed that the absorption of NO in the DBU-based N-heterocyclic DESs was governed by the chemical interaction between NO and the N atom on the N-heterocyclic compounds with the reaction stoichiometry of 1:1.
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MACROMOLECULES
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2022
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IF 6.057
Xin Qi,Lin Wang,Yingdong Zhang,Manman Jia,Liqun Zhang,Dongmei Yue
Natural rubber (NR) has a strategic position in the rubber industry due to its excellent properties, but it faces the problem of insufficient output and difficulty in recycling. Here, a high-performance elastomer was prepared by the simple epoxidation modification of bio-based Eucommia ulmoides gum (EUG). For the first time, it was found that epoxidized EUG (EEUG) with an epoxy degree of 12.3%–17.4% no longer crystallized at room temperature but had the ability to strain-induced crystallization (SIC). As a result, its vulcanizates showed excellent tensile strength (17 MPa), toughness (37.8 MJ m–3), and elasticity (strain recovery values >97%) without filler reinforcement, which is comparable with vulcanized NR. The SIC of EEUG was studied by synchrotron radiation wide-angle X-ray diffraction (SR-WAXD), and its performance was also compared with NR under the reinforcement of carbon black. In addition, through cross-linking by disulfide bonds, EEUG could be used to prepare high-performance (tensile strength of 10.5 MPa, toughness of 30.7 MJ m–3), recyclable green elastomers. This new kind of elastomer can be used as the second natural rubber, which is of great significance to solve the problem of insufficient production and difficult recovery of NR.
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ANALYTICA CHIMICA ACTA
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2022
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IF 6.911
Xin Guo,Tian Tian,Xinchun Deng,Yang Song,Xiaoming Zhou,Erqun Song
Development of rapid and accurate detection of miRNAs in complex samples is of great significance for potential early diagnosis of disease. Herein, we report a magnetic relaxation switching (MRS)-based strategy for direct detection of miRNAs in complex samples via the assistance of signal amplification system of CRISPR/Cas13a which has the ability to specifically recognize target RNA. In the designed strategy, 30 nm-magnetic nanoparticles (MB 30 ) and 1000 nm-magnetic particles (MM 1000 ) linked by single-strand RNA 1 complexes (MB 30 -RNA 1 - MM 1000 ) were employed as signal probe. After the target miRNAs (taking miR-21 as model) recognition by CRISPR/Cas13a system, the resulted trans -cleavage degrades the MB 30 -RNA 1 -MM 1000 , releasing MB 30 which caused transverse relaxation time (T 2 ) signal change. The combination of CRISPR/Cas13a assisted signal amplification and the MRS assay achieved direct detection of miR-21 in the serum sample without extracting within 60min, with a detection limit of 0.22 pM. Moreover, the detection accuracy is confirmed by performing the detection of miR-21 using qRT-PCR. The CRISPR/Cas13a system assisted MRS assay successfully achieved accurate, simple, and rapid detection of miRNAs in complex samples, showing great potential for detection miRNAs in potential clinical applications.
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高影响因子
ACS Applied Polymer Materials
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2022
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IF 4.855
Jingsheng Wang,Siqi Huo,Jun Wang,Shuang Yang,Kaiwen Chen,Chang Li,De Fang,Zhengping Fang,Pingan Song,Hao Wang
Developing bio-based flame retardants according to a green and simple strategy has drawn extensive attention recently. Hence, a biomass-derived, flame-retardant, latent curing agent (IMPA) was synthesized via the neutralization between imidazole and phytic acid in water at room temperature and was applied for single-component epoxy resin (EP). The results indicate that the shelf life of the resultant EP (EP/IMPA) increases from <1 day of the control single-component EP to 10 days at room temperature. Meanwhile, EP/IMPA features a fast curing rate at modest temperature (80–150 °C), and its gel time at 100 °C is only 14 min. Notably, EP/IMPA achieves superior flame retardancy with a limiting oxygen index of 34.7% and UL-94 V-0 rating. The peak heat release rate (PHRR), total heat release (THR), and total smoke production (TSP) of EP/IMPA are reduced by 43.0%, 31.9%, and 31.5% compared with the control sample. The enhanced fire safety is ascribed to the flame-retardant function of IMPA in both gaseous and condensed phases. Hence, this work provides a green and feasible method to create bio-based, flame-retardant, latent curing agents for one-component epoxy systems.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2022
·Vol. 33
·期 15
·12083-12092
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IF 2.779
Shen Hao,Hu Tian,Huang Huaxi,Wu Di,Xia Jianlong
Owing to the merits of solution processable, tunable electrical conductivity, high transparency and so forth, poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) has been one of the most widely used hole transport layers (HTL) in organic solar cells (OSCs), particularly in conventional cell architectures. However, the inherent acid and hygroscopic nature as well as the relatively low conductivity of the as-prepared PEDOT:PSS, seriously attenuated the stability and efficiency of the corresponding devices. To address this issue, in this contribution, the mild organic base imidazole (IM) was introduced as dopant to neutralize the acidity and improve the conductivity of the as-prepared PEDOT:PSS. Using PTB7-Th:PC 71 BM as active layer, the OSCs devices based on imidazole treated PEDOT:PSS (PEDOT:PSS-IM) shows a best of 10.09%, which is much higher than that of the un-treated PEDOT:PSS-based devices. Moreover, the PEDOT:PSS-IM-based devices display much better stability. For comparison, devices using 1-methylimidazole (MIM)-doped PEDOT:PSS as hole transport layer (HTL) has been explored. However, an inferior PCE of 8.97% was obtained. These results indicate that the hydrogen bonding interactions between imidazole and PSS plays vital role in elevating the photovoltaic performance and stability of OSCs. Additionally, PEDOT:PSS-IM also displays enhanced performance in the case of other devices with different active layers, indicating a good university in OSCs.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Jiuli Han,Haiyan Jiang,Shaojuan Zeng,Yinge Bai,Xiangping Zhang,Lu Bai
Mixed matrix membranes (MMMs) have drawn much interest in CO 2 separation due to their excellent separation performance, mechanical property, and desirable processability. However, obtaining highly compatible MMMs is a great challenge and is vital to avoid the loss of the separation selectivity of the MMMs. In this work, superbase ionic liquid (1,8-diazabicyclo[5,4,0]undec-7-ene imidazole ([HDBU][Im])) was used as a wetting agent to increase the interfacial compatibility between ZIF-67 and PIM-1, hence improving the membrane gas separation. [HDBU][Im] embeding into the MMMs could efficiently enhance the compatibility and diminish the interfacial voids. Furthermore, incorporating 5 wt% [HDBU][Im]@ZIF-67 nanocomposite into the PIM-1 matrix improves the gas permeability and CO 2 selectivity. The separation performances under the different temperatures were also conducted and showed that reducing temperature slightly decreases the gas permeability but significantly increases the CO 2 /CH 4 selectivity via enhancing the CO 2 solubility. The permeation active energies, diffusivities and solubilities were obtained to explain the gas permeate mechanism.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Meiling Lei,Jing Sun,Yu Chen,Zixian Cai,Yimin Hu
The hydrotalcites were dispersed in the hexagonal lyotropic liquid crystals (LLCs) composed of 1-hexadecyl-3-alkyl imidazolium bromide ([C 16 imC n ]Br, n = 1, 2 and 3) and H 2 O. The effects of the hydrotalcite concentration and the alkyl chain length of the [C 16 imC n ]Br on the properties and the lubricant performance of the [C 16 imC n ]Br/hydrotalcite hexagonal LLCs were studied by small angle X-ray diffraction measurements, rheology and tribology. Compared with the pure hexagonal LLCs, the incorporation of hydrotalcite into the [C 16 imC n ]Br hexagonal LLCs can increase the interlayer distances and the viscoelasticity of the hybrid hexagonal LLCs gradually. However, the friction coefficient and wear volume decrease firstly and then increase with the increasing of hydrotalcite content. With the increase of the alkyl chain length of the [C 16 imC n ]Br, the viscoelasticity, the interlayer distance and the water permeability of the mixed LLCs gradually increase which decreases the friction coefficient and wear volume at the moderate hydrotalcite content. The mechanism of the effective improvement of lubrication performance of the hybrid hexagonal LLCs is the tribofilm formed by the physical adsorption and tribochemical reaction of [C 16 imC n ]Br/hydrotalcite LLCs on the steel surface.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2022
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IF 8.025
Ling Zheng,Zilong Guo,Yinxiao Xu,Benwei Zhu,Zhong Yao
Pectate lyase (ErPL2) from Echinicola rosea JL3085 showed maximal activity at 45 °C and pH 9.0 with 0.6 mM CaCl 2 . The K m and V max values of ErPL2 for polygalacturonic sodium were 2.098 mmol/L and 0.955 mmol/s, respectively. ErPL2 endolytically degraded pectic substances into oligosaccharides with degree of polymerization (DP) 1–5. To improve the thermostability and pH operation range, recombinant ErPL2 was immobilized onto mesoporous titanium oxide particles (MTOPs). MTOPs have abundant hydroxyl groups on the surface, which is a non-toxicity and good biocompatibility carrier. The residual enzyme activity of immobilized ErPL2 at 40 °C increased remarkably from 11% to 91% compared with free enzyme. The operable pH range was extended from 8–9 to 9–11. Surprisingly, the catalytic efficiency of immobilized ErPL2 was about 19 times higher than free enzyme. To our knowledge this is the first attempt of pectate lyase immobilized on MTOPs and it provides a new option for improving the catalytic performance.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 16
·2110030
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IF 19.924
Jun He,Hongli Liu,Fei Zhang,Xianggao Li,Shirong Wang
Poor crystallinity of perovskite and extensive defects around grain boundaries are the acknowledged hindrances to obtaining high efficiency and long-term stability for organic metal halide perovskite solar cells (PSCs). Here, a 2D covalent organic framework (2D COF) nanosheets, [(TPA) 1 (TPhT) 1 ] CN , is first in situ synthesized in a PbI 2 layer with a highly crystalline structure to precisely regulate the crystallization process of perovskite in the sequential deposition method. The existence of 2D COF nanosheets can decelerate intermolecular interdiffusion and induce perovskite crystals to grow along (110) planes with enlarged grain size. Meanwhile, 2D COF nanosheets distributed around the grain boundaries reduce the defect density and promote carriers transporting in the perovskite film. The superior properties of the perovskite film afford the champion PSC device with a power conversion efficiency of 22.04%, which is over 10% higher than the control device. Moreover, the target PSC also demonstrates outstanding long-term stability. It can maintain over 90% of its initial value after 90 days storage in ambient conditions for unencapsulated devices. This work paves a new path for regulating the crystallization process of perovskites via 2D crystalline materials.
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APPLIED CLAY SCIENCE
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2022
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IF 5.907
Yang He,Lihua Zhou,Shaohua Gou,Xiaolin Qian,Zhihao Tian,Junwen Chen,Jie Liao,Jing Huo,Guangjun Gou
The imidazolium Gemini ionic liquids (IL), with alkyl groups ranging from butyl to tetradecyl as tail chains and polyoxyethylene group as linker chain, were synthesized and used as novel efficient modifiers for flexibly controlling the swelling and dispersion of Na-montmorillonite (Na Mt). The correlation between swelling behavior and structure of imidazolium Gemini IL was investigated. Too long or too short tail chains caused greater swelling, obtaining smaller particle size and reductive face-to-face stacking degree of layers. Based on the change of water contact angles, the increased stability of modified Mt in water indicated that the hydrophobicity of the tail chains played an important role in impeding the entry of water molecules into the interlayer . Zeta potential , Fourier transform infrared spectra and X-ray photoelectron spectroscopy validated the cation exchange between imidazolium Gemini IL and Na + , and confirmed the adsorption site. The molecular arrangement and intercalation were determined through adsorption behavior , interlayer space of Mt and simulation of molecular size. The imidazolium Gemini IL covered the Mt layers in monolayer, finally taking lateral (short tail chains) or paraffin (long tail chains) arrangement. The investigation will provide useful guidance for modifying Mt to obtain desirable properties and broadening the practical application of Mt hybrids.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2022
·Vol. 169
·期 2
·024502
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IF 4.386
Chao Meng,Dongmei Han,Shan Ren,Shuanjin Wang,Min Xiao,Yuezhong Meng
In the present work, a cross-linked high-temperature proton exchange membrane based on poly [2, 2'-(p-oxydiphenylene)-5, 50-benzimidazole] (OPBI), imidazole (Im) and hexachlorocyclotriphosphazene (HCCP) was prepared and characterized, aiming at their future application in fuel cell devices. The composite membranes were characterized by Fourier transform infrared (FT-IR) spectroscopy, scanning electron microscope (SEM), energy dispersive X-ray (EDX) and thermogravimetric analysis (TGA). The results show that the PBI are successfully cross-linked by the cross-linking agent, and the membranes are uniform and compact, with excellent thermal stability. Phosphoric acid (PA) doped crosslinked membranes have excellent mechanical properties and proton conductivities. The tensile strength of PA-doped PBI-ImCCP-20% at room temperature is 20 MPa, and the proton conductivity reaches 53 mS cm−1 at 160 °C without humidification. H2/O2 fuel cell assembled with PA-doped PBI-ImCCP-20% membrane delivered a peak power density of 749 mW cm−2 at 160 °C under anhydrous conditions. The excellent performance of PBI-ImCCP series cross-linked membranes makes them potential candidate for HT-PEMFC applications.
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