INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Xuan Fei,Yingjie Wang,Penglei Guo,Jinggang Wang,Guyue Wang,Guangming Lu,Weiwei Zhao,Xiaoqing Liu
Polyethylene terephthalate (PET) is one of the most widely used polymers for beverage packaging and fibers, with antimony-based catalysts currently dominating its synthesis. However, concerns about potential safety hazards associated with antimony leaching necessitate the development of environmentally benign catalysts free from heavy metals. In this work, we report the first-time utilization of Ti3C2Tx MXene as a polycondensation catalyst of PET. The intrinsic viscosity of Ti3C2Tx MXene-catalyzed PET could reach 0.78 dL/g within 2.1 h, which demonstrated a superior catalytic efficiency compared to antimony trioxide (Sb2O3). Moreover, Ti3C2Tx MXene exhibited a satisfactory performance not only in PET synthesis but also in the production of polypropylene terephthalate (PPT) and polybutylene terephthalate (PBT), thereby confirming its universality in polyester catalysis. The catalytic activity of Ti3C2Tx MXene in polycondensation reactions was attributed to the presence of strong Lewis acid sites, as supported by surface examinations and computational studies. Notably, Ti3C2Tx MXene-catalyzed PET exhibited satisfied crystallizability, as confirmed by the short crystallization half-time of only 6.9 s at 185 °C, signifying a high crystallization rate. This work highlights the potential applications of this thriving 2D material in polyester catalysis and, more importantly, provides a new perspective for the exploration and design of efficient and environmentally friendly catalyst/nucleation agents for polyester synthesis.
研究领域:
材料科学
·
催化化学
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 11
·3013-3022
·
IF 9.405
Han Hu,Ruoyu Zhang,Jinggang Wang,Wu Bin Ying,Lei Shi,Chenkai Yao,Zhengyang Kong,Kai Wang,Jin Zhu
The melt polycondensation of glycolic acid based copolymers with high molecular weights remains a big challenge. In this work, poly(butylene furandicarboxylate-co-glycolate) (PBFGA) and poly(butylene furandicarboxylate)-b-poly(glycolic acid) (PBF-b-GA) copolyesters were synthesized via melt oligomer polycondensation and melt bulk transesterification, respectively. Herein, melt oligomer polycondensation is a better method with mild preparation conditions and products with higher molecular weights (Mw). The analysis of GPC demonstrated that PBFGAs possessed a Mw of up to 8.95 × 104 g mol−1. The PBFGAs also possessed excellent thermal stability (>320 °C), which endowed the copolymers with a wider processing window than thermolabile PGA. DSC analyses displayed that PBFGA40–PBFGA10 were semi-crystalline materials that melted between 84.5 and 156 °C, while PBFGA50–60 were amorphous. Tensile tests indicated a high elastic modulus of 524–1262 MPa, tensile strength of 16–44 MPa and good elongation at break over 220% of PBFGAs, exceeding most biodegradable packaging materials. The increase of GA units slightly impacted the barrier properties, with reduced CO2 (53×) and O2 (15×) permeability coefficients than those of commercial PBAT films, and also better than those of PET. The hydrolysis of the glycolate was restrained by steric hindrance of furan rings, while in enzymatic degradation PBFGAs displayed obvious weight loss with GA units >20 mol%. With superior thermal, tensile, barrier and degradable properties, PBFGAs have the potential to serve as promising and innovative bio-based polymers for eco-friendly and sustainable plastic packaging.
研究领域:
材料科学
·
环境科学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
POLYMER DEGRADATION AND STABILITY
·
2013
·
IF 2.77
Weidong Zhou,Xiaowei Wang,Bing Yang,Ying Xu,Wei Zhang,Yajie Zhang,Junhui Ji
A series of bio-based poly(butylene adipate-co-butylene furandicarboxylate) (PBAFs) copolyesters were synthesized from 2,5-furandicarboxylic acid (FDCA), adipic acid (AA), and 1,4-butanediol (BDO) through a two-step polycondensation reaction. The copolyesters were characterized by 1 H NMR, GPC , DSC , XRD and tensile tests, and their enzymatic degradation behaviors were also investigated. They were random copolymers whose composition was well controlled and the weight average molecular weight ( M w ) ranged from 54,100 to 76,800 g/mol. By combining the results of DSC and XRD, with increasing FDCA content, PBAFs changed from semi-crystalline polymers to nearly amorphous polymers, then to semi-crystalline polymers again. Specifically, the crystallizability and melting temperature ( T m ) decreased with FDCA content 0–50 mol%, but rose again at FDCA content 75–100 mol%. And, the glass transition temperature ( T g ) increased continuously with increasing FDCA content. Consequently, the tensile modulus and strength decreased but the ultimate elongation increased at lower FDCA content (0–50 mol%), which were converse at higher FDCA content (75–100 mol%). Especially, the P(BA-40 mol% BF) shows outstanding elasticity and rebound resilience. In addition, the influences of FDCA content on the enzymatic degradation by lipase from porcine pancreas were studied in terms of the weight loss and morphological change. At FDCA content of 0–50 mol%, the copolyesters showed biodegradability but only the degradation rate of P(BA-10 mol% BF) was faster than PBA. When the FDCA content were 75–100 mol%, they were actually un-degradable. Thus, depending on their composition, PBAFs might find applications from biodegradable elastomers to thermoplastics .
研究领域:
材料科学
·
生物化学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER SCIENCE SERIES A
·
2023
·Vol. 64
·期 6
·641-652
·
IF 1
Caixia Zhao,Xu Yuan,Yang Sheng,Zou Guoxiang,Li Jinchun,Dai Junming,Pan Xiaodi
Abstract The novel flexible and resilient poly(butylene succinate- co -butylene oxybisbenzoic) esters were synthesized by a two-step reaction of esterification and polycondensation. The obtained copolyesters were characterized using gel permeation chromatography, 1 H NMR spectroscopy, wide-angle X-ray diffraction, and dynamic thermomechanical analyzer. The mechanical properties were also investigated by the tensile, cyclic tensile, creep and recovery, and stress relaxation testing. The copolyesters have the amorphous nature, excellent flexibility. The elongation at break lies in the range of 510–2870%. In addition, several theoretical models were used to describe the creep and recovery behavior of the copolyesters for a better understanding of the mechanisms.
研究领域:
高分子化学
·
材料科学
✓ 已验证
DOI
高影响因子
POLYMER DEGRADATION AND STABILITY
·
2019
·
IF 3.78
Guoqiang Wang,Yin Liang,Min Jiang,Qiang Zhang,Rui Wang,Honghua Wang,Guangyuan Zhou
Six kinds of 2,5-thiophenedicarboxylic acid-based polyesters were synthesized using a two-step melt polycondensation method from 2,5-thiophenedicarboxylic acid (TFDCA) and aliphatic diols . For all polyesters synthesized, weight-average molecular weight was higher than 1.8 × 10 4 g mol −1 . For poly(hexylene 2,5-thiophenedicarboxylate) (PHTF), poly(octylene 2,5-thiophenedicarboxylate) (POTF), and poly(decylene 2,5-thiophenedicarboxylate) (PDTF), they were crystalline polymers due to long crystallizable polyethylene-like hydrocarbon segments in the backbone. However, for poly(2-methyl-1,3-trimethylene 2,5-thiophenedicarboxylate) (PMTF), poly(neopentyl glycol 2,5-thiophenedicarboxylate) (PNTF), and poly(pentylene 2,5-thiophenedicarboxylate) (PPeTF), the melting temperature was not observed. PMTF was a brittle material (elongation at break∼2%). However, other TFDCA-based polyesters were ductile materials (elongation at break>110%). For PNTF, the highest tensile strength (∼63 MPa) and moderate elongation at break (113%) were observed, which were comparable with that of polyethylene terephthalate (PET). The polyesters prepared could be very significant for the development of bio-based polyesters.
研究领域:
材料科学
·
生物基材料
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Polymer Materials
·
2025
·
IF 4.7
ZhangHe Wang,Chao Zeng,YuHao Wu,ChaoChen Xu,ShengMing Zhang,Peng Ji,ChaoSheng Wang,HuaPing Wang
Polyester (PET) has become the focus of research in the shrink film industry due to its good heat resistance, high transparency, and excellent mechanical properties. In order to improve the shrinkage rate of the film, amorphous PET (PETG) is usually obtained by copolymerization modification using some flexible diols and so on. However, introducing flexible structures reduces the glass transition temperature (Tg) and mechanical strength, and importantly, the gas barrier properties of most PETGs are weak. Here, a series of poly(terephthalic acid-naphthalene dicarboxylic acid-ethylene glycol-neopentyl glycol) (PENTN) were prepared by melt polymerization using different contents of 1,4-naphthalene dicarboxylic acid (1,4-NDA) or 2,6-naphthalene dicarboxylic acid (2,6-NDA). The results show that the introduction of 1,4-NDA does not enhance the Tg of the copolyesters significantly, whereas the Tg of the copolyesters increases linearly with the increase in the content of 2,6-NDA. The Tg of 2,6-PENTNs ranges from 82.2 to 90.5 °C. The crystallization is inhibited effectively due to the neopentyl glycol and exhibits good transparency (>85%) and low haze value (<4%), which results in the preparation of copolyesters that are all amorphous polymers. The differences in the effects of 2,6-NDA and 1,4-NDA on the thermal properties of the copolyesters were analyzed. Meanwhile, the copolyesters were prepared into films, and the gas barrier properties were analyzed in detail. The rheological analysis reveals the free volume of the copolyester is rapidly decreasing with the introduction of the naphthalene group structure. The gas barrier property of the copolyesters can be improved to a high level. This work provides an idea for the functionalized modification of packaging materials.
研究领域:
材料科学
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Haoze Wang,Huizhe Zheng,Jie Jiang,Ling Zhao,Zhenhao Xi
Poly(ethylene glycol-co-1,4-cyclohexanedimethanol terephthalate) (PCTG) is a high-performance engineering copolyester prepared using terephthalic acid (TPA), ethylene glycol (EG), and 1,4-cyclohexanedimethanol (CHDM). In this work, a complex reaction network of PCTG copolyesters involving homopolymerization and cross-polymerization was presented and the corresponding reaction mechanism was proposed. The reaction kinetics and mass transfer behavior were investigated using static thin film experiments, wherein the variation of the hydroxyl end-group concentrations of EG and CHDM with reaction time was separately determined. The results showed that the apparent reaction rate benefited from the high temperature, thin film thickness, and high vacuum conditions. Based on the pseudosteady-state assumption, the apparent reaction rate model coupled with mass transfer was evaluated and the model parameters including the reaction rate coefficient, equilibrium constant, and mass transfer coefficient were obtained, which were further used to simulate the polycondensation process. The concentration variation of EG and CHDM, and the rate variation of each reaction during polycondensation are discussed by combining the effects of homopolymerization, cross-polycondensation, and mass transfer. The concentration of EG was more sensitive to pressure than that of CHDM, which promoted the production of CHDM at high pressures. The proposed model is expected to provide guidance for the optimization of industrial production of PCTG/PETG and generalize to other copolyester systems.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2019
·
IF 3.771
Tianzhi Bi,Zhaobin Qiu
To modify the physical properties and promote the practical application of biobased poly(butylene 2,5-furandicarboxylate) (PBF), fully biobased poly(butylene- co -propylene 2,5-furandicarboxylate) (PBPF) copolyesters with low contents (6 and 10 mol%) of propylene 2,5-furandicarboxylate (PF) units were synthesized from 2,5-dimethylfuran dicarboxylate, 1,4-butanediol and 1,3-propanediol via a transesterification and polycondensation reaction. The compositions , intrinsic viscosities , thermal stability, basic thermal parameters, crystal structures, and tensile mechanical properties of PBF and PBPF copolyesters were investigated in detail and compared with each other. Compared with those of PBF, PBPF copolyesters not only displayed high thermal decomposition temperatures (about 370 °C), slightly increased glass transition temperatures (about 40 °C), and still relatively high melting points (above 150 °C) but also exhibited the same crystal structures. The incorporation of a small amount of PF units significantly improved the tensile mechanical properties of PBPF copolyesters.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2022
·Vol. 23
·期 19
·11074
·
IF 6.208
Yanning Wang,Haicun Yang,Bingjian Li,Shi Liu,Mingyang He,Qun Chen,Jinchun Li
The main problem of manufacturing with traditional biodegradable plastics is that it is more expensive than manufacturing with polymers derived from petroleum, and the application scope is currently limited due to poor comprehensive performance. In this study, a novel biodegradable poly(butylene adipic acid/terephthalate-co-glycolic acid) (PBATGA) copolyester with 25–60% glycolic acid units was successfully synthesized by esterification and polycondensation using cheap coal chemical byproduct methyl glycolate instead of expensive glycolic acid. The structure of the copolyester was characterized by ATR-FTIR,1H NMR, DSC, and XRD; and its barrier property, water contact angle, heat resistance, and mechanical properties were tested. According to the experiment result, the PBATGA copolyesters showed improved oxygen (O2) and water vapor barrier character, and better hydrophilicity when compared with PBAT. The crystallization peaks of PBATGAs were elevated from 64 °C to 77 °C when the content of the GA unit was 25 mol %, meanwhile, the elongation at the break of PBATGA25 was more than 1300%. These results indicate that PBATGA copolyesters have good potentiality in high O2and water vapor barrier and degradable packaging material.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
·
2025
·Vol. 40
·期 2
·582-588
·
IF 1.1
Zhang Mengyi,Cheng Zhengzai,Yang Mian,Yu Qianwen,Tan Zhiping,Wandji Djouonkep Lesly Dasilva,Cheng Junpeng,Liu Panpan,Ding Ling,Gauthier Mario
High molecular weight poly(1,4-butylene 2,5-furandicarboxylate-co-isosorbide 2,5-furandicarboxylate) copolyesters (PBSIF- x ) were synthesized via melt-polycondensation of 2,5-furandicarboxylic acid (FDCA), with varying ratios of isosorbide (ISB) and 1,4-butylene glycol (BDO) catalyzed by antimony trioxide (Sb 2 O 3 ). The PBSIF -x structures were investigated using FTIR and 1 H NMR, while the GPC analysis exhibited the copolyesters molecular weights with number average molecular mass ( M n ) in the range of 11 079–15 153 g/mol. The DSC results show that PBSIF- x copolyesters have a single glass-transition temperature ( T g ) (77.45–110.96 °C), increasing with the increase in ISB content, while TGA analysis demonstrates excellent thermal stability up to 320 °C. From the thermal result, properties of PBSIF- x copolyesters are found to be within the interval of their parent homologues poly(butylene 2,5-furandicarboxylate) (PBF) and poly(isosorbide 2,5-furandicarboxylate) (PIF), which confirms the aromatic/aliphatic blending within the polymer matrix for enhanced polymer stability and performance.
研究领域:
材料科学
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
·
2021
·Vol. 36
·期 4
·557-561
·
IF 0.957
Cheng Zhengzai,Cheng Junpeng,Chen Jun,Xiong Jing,Sun Xin,Jia Ruyan,Yuan Beibei,Mario Gauthier
Terephthalic acid, 2,5-furandicarboxylic acid and 1,8-octanediol were adopted as monomers and antimony trioxide as catalyst, and poly(terephthalic acid-2,5-furandicarboxylic acid-1,8-octanediol) copolyesters identified as PEOT- x , where x is the mole fraction of furandicarboxylic acid in the samples, were synthesized by direct esterification. The molecular structure of the copolyesters was characterized by FTIR and 1 H NMR spectroscopy. Gel permeation chromatography (GPC), differential scanning calorimetry (DSC), and thermogravimetric analysis (TGA) were used to characterize the molecular weight, molar mass dispersity, glass transition temperature, and thermal stability of the copolyesters, respectively. The mechanical properties of the samples were also investigated. The number-average molecular weight ( M n ) of the samples varies from 9 700–18 800 g/mol, and molar mass dispersity ( Đ = M w / M n ) from 2.15–3.34. The initial decomposition temperature of the copolyesters is in the 332–356 °C range, with maximum decomposition rates at 390–410 °C, while the glass transition temperature ( T g ) varies from 0–33 °C. Mechanical test shows that PEOT-10 has the highest tensile strength, while PEOT-90 has the largest tensile modulus and elongation at break. The experimental results show that these copolyesters can be synthesized with relatively high molecular weights, good thermal stability, and fair mechanical properties, which makes them excellent replacements for commercial polyesters, such as PET, and these properties can be tuned through the relative amounts of biomass monomer 2,5-furandicarboxylic acid used in the reactions.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Hao Lin,Wen Li,Qingpeng Ou,Jie Liu,Zhaoyang Wei,Zhao Wang,Dean Shi,Weiwei Lei,Liqun Zhang
Biomass feedstock is an accessible alternative to finite fossil chemical resources for fabricating durable and high-performance polymers. In this study, fully biobased poly(1,5-pentylene succinate-co-itaconate-co-furanoate) (PPeSIFs) copolyesters were synthesized by using transesterification and melt polycondensation methods from dimethyl furandicarboxylate, dimethyl succinate, dimethyl itaconate, and 1,5-pentanediol. Dimethyl itaconate was incorporated to provide the cross-linkable reaction sites. Four kinds of monomers were employed to regulate the glass transition temperature and suppress crystallization. Silica/PPeSIF nanocomposites exhibited good mechanical properties, such as an ultimate tensile strength of 17.2 MPa and an elongation at break of 253%. This elastomer displayed outstanding gas barrier properties comparable to those of butyl rubber, with an O2 permeability 13 times lower than that of natural rubber. Positron annihilation lifetime spectroscopy tests demonstrated that furan moieties significantly reduced the free volume of PPeSIFs. This work provides a promising route for preparing a biobased elastomer with intrinsic high gas barrier properties.
研究领域:
材料科学
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）