ACS Applied Polymer Materials
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2024
·
IF 4.4
Shangzhong Zhang,Lifeng Yan
Direct conversion of CO2 to polymers, such as polyurea, is an effective approach for CO2 capture and utilization. However, traditional methods involving CO2 and diamine polymerization require high pressures and temperatures (>5 MPa, ∼180 °C) and result in low molecular weight polyurea. A method has been developed to synthesize polyurea directly from CO2 at mild temperature and pressure (0.1–0.5 MPa, 15–90 °C) in a one-step reaction using organic superbases as both catalysts and dehydrants with the formation of DBU-H2O. This process allows for fast polymerization (10–30 min) and yields high molecular weight polyurea (>106 g/mol). The tensile strength of the as-prepared polyurea film reaches 13.5 MPa, which indicates excellent mechanical properties.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
GREEN CHEMISTRY
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2023
·Vol. 25
·期 12
·4685-4695
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IF 9.8
Yang Wang,Huan Wang,Lan Chen,Weitao Wang,Zhaohui Yang,Zhimin Xue,Tiancheng Mu
Dissolution of lignocellulose is of significant importance for its utilization and transformation. However, it remains a great challenge to efficiently and rapidly dissolve lignocellulose under mild conditions owing to the significant lack of efficient solvents for lignocellulose dissolution. Herein, robust solvent systems were designed by a combination of ionic liquids (ILs), ethanolamine (EA), and organic superbases for the dissolution of lignocellulose. It was observed that the prepared solvents (denoted as the IL/EA-superbase) could efficiently dissolve lignocellulose at mild temperatures (below 100 °C). In particular, the EmimOAc/EA-DBN system showed the best performance, and the solubility values of Populus tomentosa, sugarcane bagasse and Miscanthus giganteus at 90 °C could reach up to 3.8%, 9.5% and 20% (g per 100 g solvent), respectively. It was revealed that EA-superbase effectively participated in the interaction between ILs and lignocellulose, thus promoting the dissolution process. A systematic study revealed that the good performance of the developed solvents toward lignocellulose dissolution resulted from the synergistic effect of the three constructed components to make the solvent have a suitable capacity for the formation of hydrogen-bonding and an appropriate microstructure.
研究领域:
生物化学
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材料科学
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DOI
高影响因子
MOLECULES
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2021
·Vol. 26
·期 6
·1735
·
IF 4.412
Fucan Zhang,Ping Liu,Kan Zhang,Qing-Wen Song
The effective separation of dimethyl carbonate (DMC) from its methanol mixture through simple, inexpensive and low energy-input method is a promising and challenging field in the process of organic synthesis. Herein, a reversible adsorption strategy through the assistance of superbase and CO2for DMC/methanol separation at ambient condition was described. The process was demonstrated effectively via the excellent CO2adsorption efficiency. Notably, the protocol was also suitable to other alcohol (i.e., monohydric alcohol, dihydric alcohol, trihydric alcohol) mixtures. The study provided guidance for potential separation of DMC/alcohol mixture in the scale-up production.
研究领域:
化学工程
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分离科学
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2014
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IF 2.613
Zhichang Liu,Pengcheng Hu,Xianghai Meng,Rui Zhang,Huiqing Yue,Chunming Xu,Yufeng Hu
Switchable polarity ionic liquids (SWILs) with low moisture sensitivity were successfully synthesized from organic amidine/fluoroalcohol and guanidine/fluoroalcohol via proton transfer reaction. The ionic liquids showed low polarity and could be converted into high-polarity fluoroalkylcarbonate ILs upon the treatment with CO 2 under mild conditions. Their high polarity state could also readily be reverted to the low polarity state by the removal of CO 2 with heating. Changes in the structures and physical properties resulting from the change from low polarity to high polarity were confirmed by NMR spectroscopy, FTIR spectrophotometry , UV–vis spectroscopy, and conductivity and miscibility measurements. These SWILs have potential applications in solute separation and solvent recovery.
研究领域:
化学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Wenjie Xiong,Mingzhen Shi,Lingling Peng,Xiaomin Zhang,Xingbang Hu,Youting Wu
CO 2 and H 2 S are considered impurities in natural gas that moderate the pace of environmental health. Developing highly efficient and cost-effective absorbents is of significance for sweetening natural gas. Herein, four superbase protic ionic liquids (SPILs) were prepared in this study. Typical physical properties (density, viscosity, and decomposition temperature) were also examined at ambient pressure. These SPILs show low viscosity values at ranging from 5.1 cP to 18.3 cP at 313.2 K. The solubility of H 2 S (0–1.0 bar), CO 2 (0–1.0 bar), and CH 4 (0–5.0 bar) was systematically measured at temperatures in the range of 298.2 K to 333.2 K. Impressively, the absolute solubility of H 2 S under 0.1 bar was found to be located at 4.31–5.15 mol/kg at 313.2 K, which is the highest value obtained among the reported results in the literature. The ideal selectivity of H 2 S/CH 4 and CO 2 /CH 4 (H 2 S or CO 2 solubility at 0.1 bar vs CH 4 solubility at 1 bar) at 313.2 K are in the ranges of 367–653 and 92.4–240, respectively. The interaction mechanism we explored was characterized by NMR and FT-IR spectroscopy. Thermodynamic parameters, such as enthalpy, Gibbs free energy, and entropy of dissolution were calculated from the temperature dependent solubility using the “deactivated model”. These SPILs are promising alternative candidates for the simultaneous removal of H 2 S and CO 2 in natural gas upgrading.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
FUEL
·
2017
·
IF 4.601
Zhaohe Huang,Bin Jiang,Huawei Yang,Baoyu Wang,Na Zhang,Haozhen Dou,Guangsen Wei,Yongli Sun,Luhong Zhang
Glycerol, an abundant byproduct in biodiesel industry process, has received a lot of attention in recent years. In this work, a series of glycerol-derived binary and ternary CO 2 binding organic liquids (CO 2 BOLs), were proposed for carbon capture. Physical properties, 1 H NMR spectra and FT-IR spectra of these systems were studied to describe the multiple interactions between constituents. The CO 2 absorption performances were evaluated in details, and excellent CO 2 uptake capacity was achieved. In order to systematically clarify the role of glycerol in superbase environment for CO 2 capture process, binary systems were further explored to support the conclusions both theoretically and experimentally. The characteristic that glycerol could easily be deprotonated in superbase environment, was proved to be benefit to the efficient and homogeneous capture of CO 2 , and a corresponding absorption mechanism was put forward. In addition, the effects of superbase and ionic liquids on absorption were also investigated. The results in this work showed how green, economic and high performance absorbents could be designed for applications of carbon capture.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
POLYMER
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2012
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IF 3.438
Minghui He,Xun Huang,Yugang Huang,Zhaohua Zeng,Jianwen Yang
The article presents a highly effective strategy for photopolymerization of acrylates via photolatent redox-accelerated reaction based on the synergistic photoinitiating systems containing photolatent superbase and readily available peroxides. Polymerization of acrylates could be instantly initiated with the effective interaction between the photogenerated amine and peroxides. Due to the persistent interaction of produced longeval amine with peroxides, remarkable post conversion after irradiation, which is significant for radiation crosslinking of photo-screened materials, was thus initially achieved in photoinitiated free radical polymerization . To explore the synergistic interactions of the photoinitiating systems, the effect of peroxide structures and QA-DBU:BPO ratios had been examined by RTIR , showing that all peroxides are applicable as the final conversion rate of acrylates is concerned. Further, BPO and CHP significantly accelerated the photopolymerization rate in air atmosphere. The synergistic efficiency of QA-DBU and BPO as a photopolymerization initiatiation system was close to that of the conventional D-1173 photoinitiator .
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
·
IF 5.3
Wentao Zheng,Qihao Pu,Shiping Wang,Xinyue Hu,Xiankun Wu
A series of low-viscous deep eutectic solvents (DESs) with superbase as HBA and amide as HBD were designed and prepared for NO absorption. Impressively, both a comparably low viscosity of 8.07 mPa∙s and a high absorption capacity of 6.43 mol∙kg −1 (∼0.19 kg/kg) at 293.2 K were achieved, which was superior to that of other reported absorbents. Through a combination of absorption experiments, FT-IR characterization, and thermodynamic modelling, the results indicated that such a high solubility for NO was originated from the mutual promotion effect between the superbase and the amide. Considering that chemical absorption occurred accompanied with physical one, a reaction equilibrium thermodynamic model (RETM) equation was derived to correlate the experiment solubility data, so that the thermodynamic parameters were obtained to evaluate the absorption process. The absorption-desorption cycle experiment revealed that the regeneration efficiency of the superbase/amide DESs could be high up to 90 %. Given the low viscosity, high absorption capacity and excellent recycle efficiency, the superbase/amide DES was considered as a promising candidate for NO capture and utilization.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2017
·Vol. 41
·期 12
·5091-5097
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IF 3.269
Zhi Wang,Zuopeng Li,Yunhe Jin,Wei Liu,Linhai Jiang,Qinghua Zhang
A series of hydrophobic room temperature ionic liquids (RTILs) composed of organic superbase-derived cations and the TFSI anion (bis(trifluromethylsulfonyl)imide) were designed and synthesized. The structures of these new RTILs were determined using 1H-NMR, 13C-NMR, IR, and elemental analysis. Their physicochemical properties, including thermal properties, density, viscosity, and electrochemical properties, were investigated. Thermogravimetric analysis (TGA) revealed that these superbase-derived RTILs have high decomposition temperatures of up to 450 °C. Studies on their electrochemical properties demonstrated that these RTILs have relatively wide electrochemical windows of up to 4.6 V and good ionic conductivities at room temperature. Their application potential as novel electrolytes in supercapacitors was also evaluated.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Polymer Chemistry
·
2022
·Vol. 14
·期 2
·172-182
·
IF 5.364
Wensheng Duan,Zhongwei Li,Zhizhou Yang,Fuyan He,Shisen Chen,Congde Qiao,Jinshui Yao,Changbin Zhang,Hui Zhao,Mei Li,Guihua Yang
In one step, two bulk chemicals of hexachlorotriphosphonitrile and 1,1,3,3-tetramethylguanidine were selected to prepare a guanidinophosphazene superbase 2,2,4,4,6,6-hexa(tetramethyl-guanidyl)-1,3,5,2λ5,4λ5,6λ5-cyclictri(phosphazene) (HTGCP, pKa of 27.2 in MeCN). The obtained HTGCP exhibits extremely high catalytic performance toward hexamethylcyclotrisiloxane (D3) in toluene and the conversion can exceed 99% under mild conditions within 10–60 min (molecular weight Mn = 10–836 kg mol−1). At high monomer dosage, Mn can be increased to 1136 kg mol−1 at 120 min. The structure and Mn of the resulting polymer have been confirmed by GPC, 1H NMR, 29Si NMR, and matrix-assisted laser desorption/ionization time-of-flight mass spectroscopy (MALDI-TOF MS). The ionic reaction between initiator and HTGCP ensures polymerization in the form of first-order reaction kinetics. Meanwhile, the polymerization rate constant increases remarkably with the increase in HTGCP concentration and the excellent linear relationship between Mn and [M]/[I] indicates well-controllable polymerization for D3. In addition, the HTGCP can still obtain high Mn for the polymerization of octamethylcyclotetrasiloxane (D4) and tetramethyl tetravinyl cyclopentasiloxane (V4), while the molecular weight distribution is relatively broad. As a superbase, HTGCP has a simpler preparation method and exhibits good application in organic polymerization under mild conditions.
研究领域:
有机化学
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高分子科学
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DOI
高影响因子
Polymer Chemistry
·
2017
·Vol. 8
·期 17
·2713-2722
·
IF 5.375
Jia Wang,Baixue Li,Dehua Xin,Rongrong Hu,Zujin Zhao,Anjun Qin,Ben Zhong Tang
The polyhydroXations, such as polyhydrothiolation and polyhydroamination, of alkynes have been well-established. However, the polyhydroalkoxylation is rarely reported. In this paper, the polyhydroalkoxylation of aromatic diynes was successfully developed in the presence of a superbase, phosphazene base (t-BuP4). A series of soluble and regio-regular anti-Markovnikov additive poly(vinyl ether)s with high molecular weights (Mw up to 40 600) were obtained in high yields (up to 99%). All the polymers are thermally and morphologically stable. The tetraphenylethene (TPE)-containing P1a2a, P1a2b and P1a2c showed unique aggregation-enhanced emission (AEE) characteristics, and their aggregates could be used for explosive detection with a superamplification quenching effect. The poly(vinyl ether)s are degradable under acidic conditions. Thus, this work not only established a new polymerization but also generated a series of functional polymeric materials that are potentially applicable in optoelectronic and biomedical fields.
研究领域:
化学
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材料科学
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高分子化学
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DOI
高影响因子
Polymers
·
2017
·Vol. 9
·期 9
·400
·
IF 3.364
Xiaoqing Dong,Peng Hu,Weizhen Shen,Zhiquan Li,Ren Liu,Xiaoya Liu
Photobase generator (PBG)-mediated thiol–epoxy photopolymerization has received widedspread attention due to its versatility in various applications. Currently, nearly all reported PBGs release amines as active species. The formed amines induce odor, yellowing, and potential toxicity. In this study, a series of novel thioxanthone-based PBGs, which were able to generate carbanion via decarboxylation under LED light irradiation, were designed and straightforwardly prepared. The formed carbanion can be used as a superbase to catalyze thiol–epoxy polymerization efficiently. Investigation on1H NMR and FT-IR confirmed the generation of carbanion intermediates. The counteranion significantly affected the photodecarboxylation efficiency. The study of photopolymerization tests, based on real-time FT-IR and dielectric analysis measurements, indicated that the generated carbanion exhibited faster polymerization rate and higher epoxy conversion than traditional superbase 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU). In differential scanning calorimeter, thermogravimetric, and nanoindentation tests, comparable thermal and mechanical properties of the photocured films catalyzed by novel PBGs were obtained. The high initiation ability combined with straightforward synthesis makes these PBGs promising candidates for commercialization.Keywords:photopolymerization;thiol–epoxy;carbanion;superbase;decarboxylation;thioxanthone
研究领域:
材料科学
·
化学工程
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DOI
高影响因子