INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Hongliang Wei,Songmao Li,Zijun Liu,Hongli Chen,Yuhua Liu,Weikun Li,Gang Wang
Herein, starch-cellulose interpenetrating network (IPN) hydrogels were fabricated by sequential Diels-Alder click reaction and photopolymerization in water. Moreover, β-cyclodextrin, a commonly used host molecule in supramolecular chemistry, was also introduced to improve the performance of the IPN hydrogel. Firstly, the starch-based dienes were synthesized by modifying starch with N-maleoyl-β-alanine, and the cellulose-based dienophiles were obtained by the reaction of cellulose and furfurylamide succinate; Secondly, the as-synthesized starch-based dienes, cellulose-based dienophiles, polymerizable β-cyclodextrin, crosslinker, and acrylamide were dissolved in water and obtained a transparent solution. The solution was maintained in a water bath of 50 °C for 3 h, forming the first network via catalyst-free click Diels-Alder reaction, subsequently, the second network was formed by photopolymerization. Their preparation conditions were optimized via one-factor experiments and their properties and structures were characterized. Finally, 5- fluorouracil (5-Fu) was used as a model drug to study the sustained release behavior of the drug-loaded hydrogels. Release profile was found to fit in Ritger-Peppas kinetic model and polymer relaxation and drug diffusion made a valuable contribution to drug release. Taking into account the virtues of easily controllable photopolymerization and catalyst-free Diels-Alder reaction, the strategy described here has a potential application in the preparation of IPN hydrogels.
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高影响因子
AICHE JOURNAL
·
2019
·Vol. 66
·期 1
·e16789
·
IF 3.463
Lun Pan,Junjian Xie,Genkuo Nie,Zheng Li,Xiangwen Zhang,Ji-Jun Zou
A one-pot Mannich–Diels–Alder reaction was developed for synthesis of high-performance jet-fuel-range spirocycloalkane with an overall yield of 71.6% from biomass and petroleum derived cyclopentanone, formaldehyde, and cyclopentadiene. HZSM-5 zeolite with Si/Al molar ratio of 130 exhibits much higher catalytic activity, along with good recycling ability. Over it, a high selectivity (81.6%) and yield (80.9%) of target adduct is achieved with almost complete conversion of cyclopentanone, attributed to the synergy effect of appropriate ratio of Lewis to Brønsted acid sites and mass transfer effect of porous zeolite. More importantly, after hydrodeoxygenation, the resultant spirocycloalkane has much higher density and volumetric neat heat of combustion (0.952 g·ml −1 , 40.18 MJ L −1 ) than the wildly used JP-10 fuel (0.936 g ml −1 , 39.41 MJ L −1 ). This work provides a promising route to produce high-performance jet-fuel-range hydrocarbons through co-conversion of biomass and petroleum derivatives.
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JOURNAL OF POLYMER SCIENCE
·
2024
·Vol. 63
·期 5
·1140-1147
·
IF 3.9
Aihemaiti Kasimu,Tianwei Hao,Wenhong Ruan,Mingqiu Zhang
In situ gel polymer electrolytes (GPEs) are promising for lithium metal batteries due to their high ionic conductivity (≈ 10 −3 S cm −1 ) and outstanding compatibility with electrode interface. However, challenges such as initiator and monomer residue, high initiation temperatures, and low mechanical properties hinder their development. To address these challenges, a low-temperature, catalyst-free method utilizing the Diels-Alder reaction between fulvene and maleimide is proposed, offering a by-product-free solution. With this method, a GPE was prepared through the Diels-Alder reaction between PEG-fulvene and bismaleimide diphenylmethane (BMI), using lithium-sulfur electrolyte (1.0 M LiTFSI in DOL (1,3-dioxolane): DME (Dimethoxyethane) = 1:1 vol% with 1.0% LiNO 3 ) as the solvent. The in situ GPE demonstrates an ionic conductivity of up to 1.11 mS cm −1 at 30°C and maintains stable cycling for 2000 h at a current density of 0.1 mA cm −2 . Furthermore, the formation of lithium dendrites is effectively suppressed. The discharge capacity of the LFP/GPE/Li battery was 118.9 mAh g −1 after 200 cycles at 0.5C, with a capacity retention of 88.20%. These results demonstrate that the in situ GPE has excellent capacity retention and cycle life, making the catalyst-free crosslinking strategy at room temperature a new plan for preparing in situ GPE. Graphical
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Weikun Li,Hongliang Wei,Yuhua Liu,Songmao Li,Gang Wang,Huayun Han
Herein, magnetic starch-based composite hydrogel microspheres (SCHMs) were produced via a Diels-Alder reaction during spray drying. The adsorption behavior of SCHMs for methylene blue (MB) was investigated systematically. The adsorption process could be described by Langmuir isothermal model and pseudo-first-order kinetic model with R 2 > 0.95 and R 2 > 0.98, respectively, resulting from its dominating physical adsorption. The thermodynamic studies showed the adsorption was spontaneous and the nature of adsorption was endothermic due to that the free energy ∆G was a negative value and the enthalpy ∆H was a positive value. The absorbent had good reusability with 90.5% of removal efficiency after 5 cycles. In addition, the effects of concentration, pH and temperature on the adsorption of MB by SCHMs were optimized using the Box-Behnken Design and response surface methodology. The order of three factors affecting the adsorption capacity of SCHMS is initial pH > initial concentration > temperature. Due to their safe, non-toxic and easily recycled advantages, SCHMs have the potential to be applied to water treatment in the future.
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高影响因子
JOURNAL OF POLYMER SCIENCE
·
2022
·Vol. 60
·期 24
·3463-3470
·
IF 3.046
Dong Xing,Jiajia Li,Miao Chen,Na Li,Xiangqiang Pan,Zhengbiao Zhang,Jian Zhu
Light-regulated polymerization has emerged as a powerful tool to control the process of polymerization. However, tuning the polymer molecular weight distribution (MWD) by light is still not well developed. Here, we present a convenient approach for controlling the MWD in reversible addition-fragmentation chain transfer (RAFT) polymerization by exploiting an ultraviolet light-induced RAFT-hetero-Diels – Alder (RAFT-HDA) reaction with a photoenol diene. The key point in this strategy is to terminate part of the propagating chains at a specific time by the RAFT-HDA reaction. In addition, a photoenol diene with a hydroxyl group is also synthesized and successfully applied to realize this strategy, which can be further utilized for chain extension of ɛ -caprolactone ( ɛ -CL) by ring opening polymerization to prepare diblock copolymers with different MWDs. Graphical
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高影响因子
LANGMUIR
·
2014
·
IF 4.384
Yan Liu,Min Tian,Huan Chang,Jinqiang Jiang,Xiangyang Yan,Zhaotie Liu,Zhongwen Liu
It is possible that the hydrophobic guest within amphiphilic polymer micelles may leak out and be captured by other species before polymer micelles adhere to the desired focus because of the complexity in an actual release procedure, rendering the reduced efficiency of the nanocarrier system. To describe such a scenario, two water-soluble fluorescent amphiphilic random copolymers of PAV and PAA with photo-cross-linkable coumarin and anthracene pendants, respectively, were chosen to investigate the equilibrating immigration and maleimide-anthracene-based Diels–Alder-trapping of hydrophobic octylmaleimide guest from one type of photo-cross-linked polymer micelles of PAV85% to another of PAA66% in aqueous solution using the emission and absorption spectra techniques.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Hongjin Kuang,Haiyang Liao,Zhanzhan Zhang,Shitao Huang,Binhui Mao,Weiyin Shan,Xiaofei Duan,Xiaolong Feng,Ting Li
High-energy-density lithium-metal batteries have garnered significant interest as an emerging class of energy storage devices. However, the intrinsic high reactivity of lithium metal introduces critical safety challenges for electrolytes (dendrite penetration and thermal runaway), severely hindering their development. This paper presents the preparation of a dynamic Diels-Alder-crosslinked metal-organic framework/poly (ionic liquid) composite electrolyte (DA-PIL/MOF) using ultraviolet (UV) curing, based on the design of furan-functionalized zirconium 1,4-dicarboxybenzene MOF (Fu-UiO-66) and maleimide-functional vinylimidazole ionic liquids (MA-IL-VI). The imidazolium cations along the PIL chains facilitate the dissociation of lithium salts. Furthermore, the incorporation of Fu-UiO-66 as a crosslinker with polymer chains establishes effective Li + pathways, thereby boosting ion transport and transference number (the ionic conductivity: 3.6 mS cm −1 at 30 °C; Li + transference number: 0.51). The incorporation of MOF into the composite electrolyte imparts flame retardancy, enhancing its thermal safety. The compact cross-linked structure ensures close contact between the electrolyte and electrodes. Additionally, the dynamic DA reaction endows the electrolyte with thermal self-healing, contributing to extended durability. Consequently, lithium iron phosphate-based cells utilizing the composite electrolyte exhibit remarkable electrochemical performance.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Bing Yan,Xu Chen,Jie Huang,Guangming Min,Zonghui Liu,Lei Shi,Bing Xue
The process of producing para -xylene (PX) from 2,5-dimethylfuran (DMF) via Diels-Alder (D-A) cycloaddition over Beta zeolites was recognized as a green and sustainable pathway for PX production. Theoretically, small zeolite particles need to be synthesized to mitigate mass transfer limitations caused by their inherent microporous structure, but particle size changes simultaneously alter crystallinity, acidity, and pore characteristics. The effects of these factors on the Diels-Alder (D-A) cycloaddition reaction have not yet been fully elucidated. In this study, Beta zeolites with average particle sizes of 100 nm, 180 nm, 450 nm, and 760 nm were prepared and applied to the D-A cycloaddition of DMF reaction. All Beta zeolites exhibited a polycrystalline structure composed of nanocrystallites and featured both micropores and mesopores. The turnover frequency (TOF) of Beta zeolite with 760 nm particle size was approximately one-third that of the other three zeolites at 160 °C, and its apparent activation energy ( E a ) for PX formation was significantly lower than that of the smaller-particle zeolites. The reduced activity and E a were primarily attributed to significant mass transfer limitation in larger-particle zeolites, with this limitation mainly originating from lengthened diffusion paths, diminished mesoporosity, mismatch in structure, and micropore alignment by internal grain boundaries. Within the particle size range where mass transfer limitations were eliminated, excessively small particle size can also detrimentally impact catalytic performance, owing to easier crystallinity reduction during the reaction.
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高影响因子
POLYMER
·
2025
·
IF 4.5
Xiaopeng Yue,Xian Shang,Jinghan Li,Lixiang Guan,Zhiwei Wang
A bio-based flame retarded thermo-reversible polymer was fabricated using furan-terminated lignin (FL) and furan-functionalized epoxidized soybean oil (FE) via Diels-Alder reaction. Two kinds of 9,10-Dihydro-9-Oxa-10-Phosphaphenanthrene-10-Oxide (DOPO) based flame retardants, including ESO ring-opening derivative (DE) and furanized reactive flame retardant (DF), were synthesized and incorporated into the networks. The incorporation of FL increased the crosslinking density, and reinforced the as-prepared FL/FE network. However, its rigid macromolecular structure also impaired the self-healing properties of network. The addition of DE and DF both improved the flame retardant properties, and they also exhibited synergistic effect during combustion. The LOI value of 80FE/10FL/5DE/5DF reached 29.3 %, and the UL-94 test also reached V-0 level. Whereas, due to the rigid molecular structure similar to lignin and the increased local cross-linking density, the incorporation of DF deteriorated the self-healing efficiency of network. On the contrary, the specimen with the incorporation of DE exhibited relative high self-healing efficiency due to the existence of hydrogen bonds. Typically, 80FE/10FL/10DE exhibited a high tensile strength (11.91 MPa), while maintained a relative high self-healing efficiency (80.45 %). These properties provide valuable insights for the practical application of bio-based polymers in sustainability and flame-retardant fields, and may have application potential in the packaging field in the future.
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高影响因子
ACS Applied Polymer Materials
·
2023
·
IF 5
Changhong Lin,Huan Ge,Puyou Ying,Tianle Wang,Min Huang,Ping Zhang,Tao Yang,Jianbo Wu,Vladimir Levchenko
Phase change materials (PCMs) can absorb and release energy while keeping the temperature constant; hence, they play a crucial role in the thermal management field. Shape-stable phase change materials (SSPCMs) were synthesized by chemical crosslinking to address the liquid leakage problem of solid–liquid phase change materials (SLPCMs) during the phase change process. However, the abandoned SSPCMs cannot be reused and recycled, which seriously restricts their practical application. Herein, a polyurethane network containing Diels–Alder bonds was used as the enclosure compound to obtain the encapsulation of polyethylene glycol (PEG), and then, the chemical structure, crystallization behavior, and phase transition ability of SSPCMs were systematically investigated. The results showed that the SSPCMs-3 sample (300 wt % PEG) had the best comprehensive performance, an enthalpy value of 171.7 J/g, and no leakage at 80 °C for 1 h. Moreover, the structure, crystallization behavior, and phase transition ability of SSPCMs could also basically remain unchanged after multiple thermal cycling and reprocessing.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Ying Liang,Meng Xia,Yuxiang Zhao,Dong Wang,Yongpeng Li,Zhuyin Sui,Juanxiu Xiao,Qi Chen
The development of functional covalent organic frameworks (COFs) with specific properties is an emerging research field. In the current work, COF-SQ-Ph was synthesized through the aza-Diels-Alder reaction between phenylacetylene and the matrix COF-SQ (triazine-based COF) generated from the organic monomers 2, 4, 6-tris(4-aminophenyl)-1, 3, 5-triazine and 2, 5-dimethoxyterephthalaldehyde in flask. The functionalized COF-SQ-Ph with an extended π-conjugated structure and enhanced structural stability was used as the sulfur loading recipient to prepare sulfur cathodes for lithium-sulfur batteries. Sulfur-impregnated COF-SQ-Ph marked as COF-SQ-Ph-S displayed better cycling stability with a specific capacity of 618 mA h g −1 after 150 cycles due to the lithiophilic interaction between lithium polysulfides and nitrogen atoms from quinoline and triazine moieties in COF-SQ-Ph-S. The functionalization of triazine-based COFs through a cycloaddition reaction in flask could promote the large-scale preparation of tailored COFs and the post-synthesis modification of COF-SQ.
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高影响因子
PROGRESS IN ORGANIC COATINGS
·
2020
·
IF 4.469
Jingcheng Liu,Zhen Zhou,Xunzheng Su,Jiancheng Cao,Mengjia Chen,Ren Liu
A series of multi-crosslinkable, self-healing coatings were developed to enhance the mechanical properties through tandem UV-curing and Diels-Alder (DA) chemistry. First, multi-arm UV-cured polyurethane (PU) pre-polymers (IPxH 12 ) were prepared based on cyclotriphosphazene monomer (H 12 ) with more benzene ring structure and half-blocked photosensitive oligomer. Then N, N'-(4, 4′-methylenediphenyl) bismaleimide (BMI) and furfuryl alcohol (FA) were used as the raw materials to prepare DA intermediate by Diels-Alder reaction. The DA intermediate was further reacted with methacrylic acid isocyanate (IEM) to obtain the modified I DA monomer (UV curable DA monomer, containing acrylic double bond). The structure of IPxH 12 and I DA was characterized by FT-IR and 1 H-NMR. UV-cured self-healing coatings were prepared by designing some coating formulations with the IPxH 12 , I DA and initiator. The self-healing properties and mechanical properties of the coatings were investigated. The results revealed that the hardness of the coating was up to 3H, and the introduction of I DA improved its self-healing performance, when the ratio of DA monomer to PU was 2:1, the repair effect was the best. The UV-curable self-healing coating has potential application in metal protection and other fields.
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