CHEMISTRY & BIODIVERSITY
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2023
·Vol. 20
·期 8
·e202300350
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IF 2.9
Mengyi Ba,Ruonan Chen,Qiuchen Huang,Yanli Song,Wen Li,Yuanyuan Zhang,Haixin Liu,Xiang Xu,Weidong Zhang,Zhiqiang Cai,Tao Sun
This work firstly reported a new polycaprolactone based material functionalized with guanidinium ionic liquid (PCL-GIL) as the stationary phase with high resolution performance for capillary gas chromatography (GC). It is composed of polycaprolactone (PCL) and guanidinium ionic liquid (GIL) with amphiphilic conformation. The PCL-GIL capillary column coated by static method exhibited high column efficiency of 3942 plates/m and moderate polarity. As a result, the PCL-GIL column exhibited high-resolution capability. For a mixture of 27 analytes with a wide ranging polarity and outperformed the PCL-2OH and HP-35 columns, showing its advantageous separation capability for analytes of diverse types. Moreover, the PCL-GIL column showed high resolving capability for various positional isomers and cis-/trans- isomers, including alkylbenzenes, chlorobenzenes, naphthalenes, bromonitrobenzenes, chloronitrobenzenes, benzaldehydes, phenols, alcohols, respectively. In a word, PCL derivatized by GIL units as a new type of stationary phase has a promising future in GC separations. Graphical
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yijia Yu,Shengjie Liu,Wenjuan Xia,Zhichen Zhu,Wenjin Wang,Chuanjiang Zhou,Zhaoqiang Wu,Hong Chen
To meet the development of multifunctional surfaces with long-term antibacterial activity for biomaterials and implantable devices, herein, a novel self-polishing antibacterial surface was developed. The functionalized surface was prepared by first surface-initiated ring-opening grafting polymerization (SI-ROP) of a cyclic carbonate monomer 4′-(fluorosulfonyl)benzyl-5-methyl-2-oxo-1,3-dioxane-5-carboxylate (FMC) containing a sulfonyl fluoride group in the side chain onto the material surface and then by a “sulfur(IV)-fluorine” exchange (SuFEx) postclick modification reaction to link the imidazolium salt ionic liquid to the polyFMC (PFMC) brush. In vitro experimental results showed that the functionalized surface has good biocompatibility, enzymatic biodegradable properties and excellent bactericidal properties, which can effectively kill E. coli (∼94%) and S. aureus (∼93%). In addition, the functionalized surface can release the killed bacteria (∼90%) several times efficiently under the action of lipase enzymatic degradation, restoring the original bactericidal function of the surface, thus forming a dynamic self-polishing and self-renewing antibacterial surface. Therefore, this method for the fabrication of self-polishing antibacterial surfaces may offer innovative insights into applications of biomedical implant materials.
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LANGMUIR
·
2023
·
IF 3.9
Jinmeng Zhu,Jinghan Ding,Yuke Li,Qi Wang,Fan Yang,Cong Jia,Yaxu Zhang,Xichen Zhao,Wenqiang Dong,Jia Wang,Zhiyong Lu,Xuanhua Li
After decades of research in the conservation of cultural heritage, nanolime (NL) has emerged as a potential alternative inorganic material to the frequently used organic materials. However, its poor kinetic stability in water has been a major challenge that restricted its penetration depth through cultural relics and resulted in unsatisfactory conservation outcomes. Here, for the first time, we realize NL water dispersion by modification of ionic liquid (1-butyl-3-methylimidazolium tetrafluoroborate) via a sample aqueous solution deposit method. Our findings indicate that the cation of the ionic liquid (IL) binds strongly to the surface of NL particles (IL-NL) by forming hydrogen bonds with Ca(OH)2 facets. The absorption of IL causes an unexpected significant alteration in the morphology of NL particles and results in a drastic reduction in NL’s size. More importantly, this absorption endows NL excellent kinetic stability dispersed into water and implements NL water dispersion, which makes a breakthrough in terms of extreme poor kinetic stability of as-synthesized NL and commercial NL in water. The mechanism driving IL-NL water dispersion is explained by Stern theory. In the context of consolidating weathered stone, the presence of IL may delay carbonation of NL but the penetration depth of IL-NL through stone samples is three times deeper than that of as-synthesized and commercial NLs. Additionally, the consolidation strength of IL-NL is similar to that of as-synthesized NL and commercial NL. Moreover, IL-NL has no significant impact on the permeability, pore size, and microstructure of consolidated stone relics. Our research contributes to the field of NL-related materials and will enhance the dissemination and utilization of NL-based materials in the preservation of water-insensitive cultural heritage.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lurong Ge,Yaohui Feng,Yanjun Dai,Ruzhu Wang,Tianshu Ge
Composite sorbents with hygroscopic salts (like LiCl and CaCl 2 ) impregnated porous matrixes obtained special attention in the past years, especially for solid desiccant dehumidification. However, the drawback of strong corrosivity limited their practical implementation. Alternatively, ionic liquid (1-ethyl-3-methylimidazole acetate) with less corrosivity is confined into ordered mesoporous MCM-41 to fabricate composite sorbent in this study, overcoming the poor mass transfer or limited adsorption capacity of single sorbent. Comprehensive characterizations including SEM, TEM, XRD, FTIR and N 2 adsorption prove that the ionic liquid is encapsulated in ordered channels of MCM-41. Sorption isotherms and kinetics indicate that the composite sorbent has superior water sorption performance (0.5 g/g at 20 °C/70 % RH), fast sorption rate under wide humidity range and potential of low temperature-driven regeneration. Moreover, the leakage test and corrosion experiment reveal that the composite sorbent has long-term stability and is corrosion-free to metal components. Further, the dehumidification performance using desiccant coated heat exchanger with reported composite sorbent is evaluated, showing 5 times higher dehumidification capacity than that of MCM-41 and 2 times higher than traditional silica gel (typical ARI summer, 35 °C, 40 % RH). This study identifies a feasible way of using ionic liquids to develop energy-efficient, safety-ensured and low-cost composite sorbents for water sorption-related applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Qiuying Li,Rui Zhang,Yaxing Li,Xianghai Meng,Haiyan Liu,Xiaowen Wang,Chunming Xu,Haifeng Dong,Qian Su,Xiangping Zhang,Zhichang Liu
Alkylation performance of isobutane with propene catalyzed by composite ionic liquid (CIL) was deeply investigated. Critical components of alkylate were C7 isoparaffins, which were mainly 2,3-dimethylpentane and 2,4-dimethylpentane. The optimal reaction conditions were as follows: reaction temperature of 15 °C, reaction time of 5 s, stirring rate of 1500 rpm, IL/HC ratio of 1.0, and I/O ratio of 68. Under these conditions, the yield of C7 isoparaffins was 78.9 wt %, and the research octane number of alkylate was 86.2. The reaction mechanism and pathway of isobutane/propene alkylation were proposed on the basis of component distribution. C7 isoparaffins were mainly from direct alkylation, and C8 isoparaffins were mainly from disproportionation. Compared with traditional concentrated sulfuric acid and hydrofluoric acid catalysts, more direct alkylation and less self-alkylation occurred, and the yield of propane was much lower when CIL was used. It was also proved that propene could be used in the CIL-catalyzed alkylation industrial unit due to the low propane production.
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POLYMER DEGRADATION AND STABILITY
·
2022
·
IF 5.204
Zhiqiang Jiang,Dongxia Yan,Jiayu Xin,Fei Li,Mengquan Guo,Qing Zhou,Junli Xu,Yufeng Hu,Xingmei Lu
The methanolysis of polyethylene terephthalate (PET) was investigated using poly(ionic liquid)s (PILs) synthesized with 1-vinyl-3-ethylimidazole acetates ([VEIm]Ac) and acrylic acid metal salts, and the activities of the PILs were screened. The effects of reaction temperature, reaction time, methanol amount, catalyst amount and PET sources on the methanolysis of PET were investigated using the optimized catalyst PIL-Zn 2+ . Under the optimal conditions the conversion of PET was 100% and the yield of dimethyl terephthalate (DMT) was 89.1%. In addition, the catalyst has very good applicability for methanolysis of different PET raw materials. More importantly, the PIL-Zn 2+ catalyst could be recycled by simple filtration after the reaction, and could be reused six times without significant decrease in PET conversion and DMT yield. The catalysts were analyzed by TGA, FT-IR, XRD and ICP before and after recycling, the results showed no change in the structure of the catalyst, reflecting the good stability of the catalyst. The reaction kinetics of PIL-Zn 2+ was first-order with an activation energy of 107.6 kJ/mol. This work mainly provides a way to design efficient, stable and recyclable catalysts for PET methanolysis.
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BIORESOURCE TECHNOLOGY
·
2022
·
IF 11.889
Hailian Gao,Jiebin Wang,Meixuan Liu,Shunxin Wang,Wenbo Li,Qingda An,Kunlan Li,Ligang Wei,Chi Han,Shangru Zhai
The aerobic oxidation of lignin model 2-phenoxyacetophenone (2-PAP) in cooperative ionic liquid mixtures (CoILs) with 1-ethyl-3-methylimidazolium acetate ([C 2 C 1 im]OAc) and 1-benzyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([B Z C 1 im]NTf 2 ) was investigated. Complete degradation of 2-PAP was achieved with [C 2 C 1 im]OAc/[B Z C 1 im]NTf 2 molar ratio ( R IL ) of 1/1 and 1/2 at 100 °C for 2 h. The conversion and product yields from CoILs were higher than those in pure ILs, indicating the cooperative effects of [C 2 C 1 im]OAc/[B Z C 1 im]NTf 2 on cleaving aryl–ether bonds. [C 2 C 1 im]OAc promoted the catalytic cleavage of aryl–ether bonds and solvation, and [B Z C 1 im]NTf 2 induced the formation of alkyl radicals and enhanced the product selectivity. Accordingly, the highest conversion of alkali lignin (79.8%) was obtained with R IL of 5/1 at 100 °C for 2 h, and phenol monomers (306 mg/g) were selectively produced. The CoILs exhibited good catalytic capacities for oxidative depolymerization of lignin, which strongly depends on the changes in intermolecular interactions and structural organization with varying R IL .
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RSC Advances
·
2022
·Vol. 12
·期 7
·4408-4416
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IF 4.036
Guanhao Liu,Jingyi Yang,Yibo Zhao,Xinru Xu
Novel modified MOF intercalated hydrotalcites was synthesized for catalyzing the conversion of glycerol into high value-added glycerol carbonate in this paper. [APmim]OH/ZIF-8 was prepared by encapsulating aminopropyl hydroxide imidazole ionic liquid in ZIF-8 and inserted in Ca–Mg–Al hydrotalcites with layered structures to prepare [APmim]OH/ZIF-8/LDH with strong basicity and high specific surface area. ZIF-8, [APmim]OH/ZIF-8 and [APmim]OH/ZIF-8/LDH were characterized by XRD, FT-IR, SEM and nitrogen adsorption–desorption. The results showed that the conversion rate of glycerol can reach 98.6% and the glycerol carbonate yield was 96.5% in the transesterification of glycerol with dimethyl carbonate catalyzed by [APmim]OH/ZIF-8/LDH when the molar ratio of DMC and glycerol was 3 : 1, the catalyst dosage was 3 wt%, the reaction temperature was 75 °C and the reaction time was 80 minutes. The glycerol conversion rate can still reach more than 90% after five reaction cycles.
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INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Zeyu Zhang,Guiquan Jiang,Jiuyin Pang,Ling Su
In this paper, acrylate and glycidyl methacrylate (GMA) were grafted onto the main chain of soy protein isolate (SPI) in 1-butyl-2,3-dimethylimidazole chloride ionic liquid ([BDMIM][Cl]), to prepare a renewable soy protein graft copolymer via atom transfer radical polymerization (ATRP). The effect of unfolding degree of soy protein structure on pretreated SPI was studied via Fourier-transform infrared spectroscopy (FT-IR), hydrogen nuclear magnetic resonance spectroscopy (1 H NMR), surface tension (ST) and contact angle (CA) measurements. The results of FT-IR, 1 H NMR and energy dispersive spectrometry (EDS) indicated the successful synthesis of 2-bromoisobutyryl-functionalized SPI.The analysis of FT-IR and 1 H NMR spectra showed that the soybean protein graft copolymer was successfully synthesized. In addition, the grafting of acrylate onto soybean protein enhanced the hydrophobicity of the copolymer, and the static contact angle was above 90°. Differential scanning calorimetry (DSC) analysis revealed that the thermal stability of pretreated SPI was reduced. The new glass transition temperature in the copolymers also proved the successful synthesis of the copolymers. The tensile strength of the carbon fiber multifilament infiltrated with the copolymers was improved, indicating their potential application in the reinforcement of carbon fiber material.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2023
·
IF 2.6
Yong Peng,Yanhao Shen,Qi Huang,Xiaoqing Yang,Yuqing Yang,Jing Zhong,Jiawen Pan,Xiaoyu Han
Acetic acid aqueous solution is a common and typical near-boiling mixture in the petroleum, chemical, polymer, pharmaceutical and food industries. Because of the large number of ideal plates for separating acetic acid and water by ordinary distillation, the energy consumption and production cost are high. Designable ionic liquids (ILs) and deep eutectic solvents (DESs) are environmentally-friendly entrainers for extractive distillation. Many azeotropic systems enhanced by adding ILs or DESs have been studied, but the near-boiling water/acetic acid system is rarely discussed. In this study, an IL 1,2,3-trimethylimidazolium dimethylphosphate ([TMIM] + [Me 2 PO 4 ] − ) with easy synthesis, low production cost and good thermal stability was employed as the rectification entrainer for water/acetic acid system, while the DESs were easy to react in acetic acid aqueous solution and was abandoned. First, the relative volatility of water (1) and acetic acid (2) at the more difficult separation point ( x 1 ′ = 0.9) was measured using a modified Othmer still at 101.32 kPa. When the mole fraction of entrainers was 0.071, these relative volatilities were 2.80 ( n , n -dimethylformamide), 2.88 (1-methyl-2-pyrrolidinone), 4.82 ([TMIM] + [Me 2 PO 4 ] − ) respectively. The separation performance of [TMIM] + [Me 2 PO 4 ] − was 67% higher than that of 1-methyl-2-pyrrolidinone. Then, the effect of [TMIM] + [Me 2 PO 4 ] − concentration on the relative volatility was investigated. The relative volatility was dramatically increased from 1.60 to 6.85 with 0–0.103 mol fraction of [TMIM] + [Me 2 PO 4 ] − and was 4.28 times that in an IL-free system. After that, isobaric vapor–liquid equilibrium (VLE) data of water + acetic acid, water + [TMIM] + [Me 2 PO 4 ] − and water + acetic acid + [TMIM] + [Me 2 PO 4 ] − ([TMIM] + [Me 2 PO 4 ] − at ∼ 5, 15, and 25 mass%) systems were determined at 101.32 kPa. Also, Based on the chemical theory and Hayden–O’Connell method, the binary energy parameters of the NRTL (Non-Random-Two-Liquid) model for these systems were regressed and the predicted values were found to fit the experimental VLE data quite well.. For the first time, we have found that [TMIM] + [Me 2 PO 4 ] − as an entrainer is superior to conventional volatile solvents for water/acetic acid distillation in terms of performance, which provides more choices and imagination for industry. At the same time, it promotes understanding of the influence of IL structure on water/acetic acid separation performance, and is also an important inspiration for the distillation of other near-boiling systems.
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ENERGY & FUELS
·
2023
·
IF 5.3
Ruiqing Zhang,Ziwei Zhai,Li Wang,Sibao Liu,Guozhu Liu
Catalytic cracking–dehydrogenation of hydrocarbon fuels with hydrocarbon-soluble metal nanoparticles is an appealing way to improve fuel heat sink in a high-speed aircraft. In this work, two hydrocarbon-soluble metal nanoparticles (Pd@ILs and Pt@ILs) by using symmetrical imidazolium ionic liquids (1,3-bis(14-alkyl) imidazolium bromide) as protective agents were successfully synthesized. The catalytic performance for cracking and dehydrogenation of decalin-based nanofluids was investigated using an electrically heated tubular reactor. In comparison with Pd@14N with the conventional tetradecylamine ligand, Pd@ILs and Pt@ILs catalysts exhibited smaller average particle sizes and showed better performance in terms of dispersion stability, thermal stability, and catalytic activity. Fourier transform infrared (FT-IR) and density functional theory (DFT) calculations demonstrated that the strong affinity of C atoms in the conjugate imidazole ring to the metal surface allows these nanoparticles to be stably dispersed in decalin for at least 2 months. In the quasi-homogeneous conversion of decalin, Pd@ILs exhibited the best performance in promoting fuel cracking and dehydrogenation conversion with the highest yields of hydrogen and unsaturated hydrocarbon products, especially aromatic products, thus enhancing the heat sink of nanofluids. Particularly, the heat sink of nanofluids with the Pd@ILs catalyst was 3.39 MJ kg–1 at 700 °C, which was 0.58 MJ kg–1 higher than that from decalin thermal cracking and 0.43 MJ kg–1 higher than that of the nanofluids with the Pd@14N catalyst. In addition, Pd@ILs nanofluids gave the highest heat sink of 3.61 MJ kg–1 at 725 °C. The significant enhancements are attributed to cooperative interplay between the initiation effect of ILs and the remarkable catalytic ability of Pd nanoparticles in cracking–dehydrogenation reaction, as well as the unique properties of Pd@ILs, including smaller Pd particle size, more accessible surface Pd active sites, and higher thermal stability. This work shows that symmetrical imidazolium ionic liquid-capped metal nanoparticles can serve as effective quasi-homogeneous catalysts for enhancing heat sink of hydrocarbon fuels through catalytic cracking and dehydrogenation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Yuanchao Pei,Yajuan Niu,Wanjun Zhang,Yaxin Zhang,Jie Ma,Zhiyong Li
Tunable microstructure of microemulsion self-assembly systems has the prominent application as nanoreactors in reaction processes. Scientific and technological interest in microemulsions derived from the confinement effect of polar or nonpolar domains for hydrophilic/hydrophobic molecules. Benefiting from the tunable nature, ionic liquids-based self-assembly systems have been demonstrated as a versatile platform for catalytic reaction , drug delivery, functional materials fabrication and among others. In this work, ionic liquids microemulsions were designed by using ionic liquids as apolar phase and surfactant . The phase equilibrium and microstructure were studied through phase diagram , conductivity method and dynamic light scattering . Ionic liquids-in-water microemulsions were proposed as nanoreactor for fabrication of nanosized platinum/titanium dioxide composites. The size, morphology and catalytic performance can be tuned by the microemulsion structure through its confinement effect. The hydrolysis of ammonia borane catalyzed by these composites exhibits better catalytic activity with higher turnover frequency and lower activation energy of the reaction. It is believed that the nanoreactors constructed from versatile ionic liquids will provide new guidance in designing advanced scientific applications.
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