JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2021
·
IF 6.064
Xiaoling Qu,Guangyuan Zhou,Rui Wang,Haiyan Zhang,Zhipeng Wang,Min Jiang,Jun Tang
In pursuit of poly(ethylene 2,5-furandicarboxylate) PEF materials with high molecular weight, satisfactory appearance and faster crystallization rate, its preparation from dimethyl furan-2,5-dicarboxylate (DMFD) with ethylene glycol (EG) in the trace presence of metal zinc was performed via transesterification method. Optimization of the main polymerization parameters enabled Zn-catalyzed PEF to gain high molecular weight ( M n , 5.40 × 10 4 g mol −1 ) and low content of diethylene glycol furandicarboxylate unit (DEGF, 2.91%). On the basis of experimental phenomena and high performance liquid chromatography (HPLC), the actual catalytic active species of metal zinc in the polymerization was speculated to be a salt of 2, 5-furandicarboxylate derivative (Zn(II)). The in-stiu catalyst can efficaciously inhibit the influence of by-product FDCA on the color of PEF, which displayed quite better appearance (close to white). Differential Scanning Calorimetry (DSC) showed that the in-stiu catalytic system acted as nucleating agent (NA) and the crystallization half-time (t 1/2 ) of PEFs-Zn was only 1/4 of that of PEF-tin. Additionally, series of high molecular weight furan-based polyesters from DMFD and diols with different methylene (3, 5, 6 and 8) were obtained by zinc powder as in-stiu catalyst, which further evidenced it to be efficiency and universality.
研究领域:
材料科学
·
聚合物化学
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2019
·Vol. 12
·期 22
·4927-4935
·
IF 7.804
Xiao-ling Qu,Min Jiang,Bing Wang,Jin Deng,Rui Wang,Qiang Zhang,Guang-yuan Zhou,Jun Tang
Graphical Low loading : With a small catalyst loading of metal-free and selective ionic liquids (0.1 % based on 2,5-furandicarboxylic acid), bioderived poly(ethylene 2,5-furandicarboxylate) is efficiently prepared with high molecular weight by the electrophilic activation induced by hydrogen bonds, which are formed between the ionic liquid [C 2 MIM] + and the carbonyl oxygen. Green synthesis of bioderived high-molecular-weight poly(ethylene 2,5-furandicarboxylate) (PEF) over metal-free catalysts is a significant challenge. This study focuses on PEF prepared from ethylene glycol and 2,5-furandicarboxylic acid (FDCA) through a direct esterification method with ecofriendly metal-free ionic liquids (ILs) as catalysts. The catalytic activities of a series of imidazolium cations in the presence of various anions are systematically investigated and found to be mainly governed by the anions. Among the ILs studied, 1-ethyl-3-methylimidazolium tetrafluoroborate ([C 2 MIM]BF 4 ) is identified as the best catalyst, showing excellent catalytic activity, selectivity, and stability, even at low catalyst loadings (0.1 mol % w.r.t. FDCA). Optimization of the polymerization parameters enables [C 2 MIM]BF 4 -catalyzed production of PEF with a high number-average molecular weight ( M n =5.25×10 4 g mol −1 ). The relationship between Brønsted acidity and catalytic activity is also investigated and the results show that the trend in catalytic activity is in good agreement with that in Brønsted acidity, as determined by the Hammett method. Additionally, on the basis of experimental results and density functional theory calculations, an electrophilic activation mechanism induced by hydrogen bonds is proposed. This strategy of adjustable acidity and anion structure in ILs provides an opportunity to develop other ILs for bio-based polyesters through green synthesis pathways.
研究领域:
化学工程
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材料科学
·
绿色化学
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2022
·Vol. 24
·期 13
·5181-5190
·
IF 11.034
Jing Yi,Yuxuan Li,Yuhao Zhao,Zhanwei Xu,Yuanpeng Wu,Min Jiang,Guangyuan Zhou
In recent years, a large number of studies have been performed on the modification of poly(ethylene 2,5-furandicarboxylate) (PEF), focused on improving its brittleness and crystallization rate. Here, we present a series of biobased copolyesters synthesized from 2,5-furandicarboxylate (FDCA), ethylene glycol (EG) and (5,5′-((phenethylazanediyl)bis(methylene))bis(furan-5,2-diyl))dimethanol (PhDM) via green and mild routes. The introduction of PhDM into the PEF backbone not only alters its thermal properties and mechanical properties, but also endows it with UV shielding performance and regulatable gas barrier properties. DSC analysis showed that the copolyesters were amorphous. Compared with PEF, the copolyesters achieved better thermal stability and the initial thermal decomposition temperature was increased by 8–41 °C. The tensile testing demonstrated that the copolymers possessed significantly improved elongation at break (εb = 15%–35%) compared with PEF (εb = 5%). Obviously, the copolyesters with 30 mol%, 40 mol% and 50 mol% PhDM could shield ∼100% UV light and all copolyesters exhibited good transparency in the visible region. Inherently, the O2, CO2 and water permeability coefficient (P) values of the copolymers increased with increasing PhDM content, and the CO2/O2 selectivity (α) value first increased and then decreased. The copolymer film that contains 30% PhDM (mol/mol), and shows high CO2/O2 selectivity (α = 6.8) in comparison to PEF (α = 1.3) and polypropylene (PP) (α = 3.3), was selected to test its food preservation ability with fresh winter jujube. Winter jujube packed with PhDM can be preserved for one week without deterioration, compared with the winter jujube packed with PEF, which has obviously rotted. These results indicate that the copolymer is a promising packaging material for fresh fruit preservation.
研究领域:
材料科学
·
食品科学
·
高分子化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）