JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 25
·11325-11338
·
IF 3.553
Cao Ying,Zhang Jiatian,Zhang Dandan,Lv Yan,Li Jie,Xu Yiting,He Kaibin,Chen Guorong,Yuan Conghui,Zeng Birong,Dai Lizong
Hexagonal boron nitride (hBN), as one of the two-dimensional (2D) materials, possesses many excellent properties like others. Herein, we report a novel self-healing epoxy filled with hBN. High compatibility between hBN and the epoxy matrix was obtained by the modification of hBN with silane coupling agent (Mi-Si). At the meantime, excellent self-healing behavior was achieved by retro Diels–Alder (r-DA) reaction between the maleimide functional group in the modified hBN (m-hBN-OH) and the added furfurylamine. Besides, the inadequate curing of epoxy led to the glass transition temperature (Tg), which is also seemed as the transition temperature for the shape memory of the epoxy, below the r-DA reaction temperature, and endowed the system with the shape memory-assisted self-healing properties. The m-hBN-OH was characterized by Fourier transform infrared spectra, nuclear magnetic resonance ( 1 H-NMR) spectra, X-ray diffraction experiments, X-ray photoelectron spectroscopy measurements and so on. The new m-hBN-OH modifier was prepared with the optimized Mi-Si/hBN-OH weight ratio of 3.0, which could both improve the thermal property and achieve better thermal conductivity. This designed m-hBN-OH/epoxy could actually show ideal self-healing properties due to the shape memory-assisted self-healing effect. The thermal conductivity of the neat epoxy resin and the m-hBN-OH/epoxy was 0.2156 W m −1 K −1 and 0.4358 W m −1 K −1 , respectively. As a novel material with efficient thermal conductivity, hBN made great contribution to the thermally induced shape memory and self-healing property. Systematic researches reveal that the composites are promising as long durable thermal interface materials, anti-scratch materials and so on.
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MATERIALS CHEMISTRY AND PHYSICS
·
2017
·
IF 2.084
Xiangcheng Liu,Qing Wan,Zhe Zhao,Jinglong Liu,Zhuoyong Zhang,Fengjie Deng,Meiying Liu,Yuanqing Wen,Xiaoyong Zhang
Fluorescent nanodiamond (FND) has received increasing research interests for bioimaging and drug delivery owing its outstanding physicochemical properties and low toxicity. However, synthesis of FND in large scale with desirable optical property is still a big challenge. In this work, we reported for the first time that non-fluorescent ND can be facilely converted into FND through surface modified with aggregation-induced emission fluorophore containing luminescent polymers through the microwave-assisted typical Diels-Alder (D-A) reaction. The final FND (named as ND-poly(Phe-PEGMA-IA)) displayed extensive fluorescence, high water dispersibility and desirable biocompatibility. Cell imaging results demonstrated ND-poly(Phe-PEGMA-IA) exhibited great stain performance. Furthermore, anticancer drug (cisplatin, DDP) can be effectively loaded onto ND-poly(Phe-PEGMA-IA) and controlled release it under acidic environment. All of these favorable properties endow ND-poly(Phe-PEGMA-IA) great potential for biological tracing and controlled drug delivery. Taken together, we have developed a microwave-assisted D-A reaction for preparation of multifunctional FND with great potential for biological imaging and controlled drug delivery applications.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Yongli Shi,Suyue Xu,Jingya Zhao,Huiqing Zhu,Xiaofei Pan,Bingqian Zhao,Zeyu Sun,Na Li,Xueyan Hou
The objective of this study was to develop an injectable hydrogel based on furfuryl amine-conjugated hyaluronic acid (FA- conj -HA) and evaluate the in vivo anti-4 T1 tumor activity of doxorubicin-loaded hydrogel (DOX@FA- conj -HA gel ). The cargo-free hydrogel (FA- conj -HA gel ) was fabricated through a Diels-Alder reaction at 37 °C with FA- conj -HA as a gel material and four armed poly(ethylene glycol)2000-maleimide (4-arm-PEG2000-Mal) as a cross-linker. The bio-safety of FA- conj -HA gel were assessed, and the in vivo antitumor activity of DOX@FA- conj -HA gel was also investigated. Many 3D network structures were observed from scanning electron microscope (SEM) photograph, confirming the successful preparation of FA- conj -HA gel . The absence of cytotoxicity from FA- conj -HA gel was proved by the high viability of 4 T1 cells. In vivo bio-safety studies suggested that the obtained FA- conj -HA gel did not induce acute toxicity or other lesions in treated mice, confirming its high bio-safety. The reduced tumor volumes, hematoxylin-eosin staining (H&E), and TdT-mediated dUTP-biotin nick end labeling (TUNEL) analysis indicated the potent in vivo anti-4 T1 tumor effects of DOX@FA- conj -HA gel . In conclusion, the favorable bio-safety and potent antitumor activity of DOX@FA- conj -HA gel highlighted its potential application in oncological therapy.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Xianlong Liu,Yiting Zhao,Gewei Zhang,Chengxiang Shi,Lun Pan,Xiangwen Zhang,Ji-Jun Zou
Attention has been drawn to the potential of renewable biomass as an alternative to petroleum-based feedstocks for the synthesis of high-density fuels given the depletion of petroleum resources and critical environmental issues. In this study, fused ring high-density liquid fuel precursors were directionally synthesized from biofuran derivatives by the Diels–Alder reaction. The impact of different dienophiles on the Diels–Alder reaction of 2-methylfuran facilitated by zeolites was evaluated. The influences of the catalyst, reaction temperature, and reactant ratio on the reaction were explored. Moreover, this study emphasized the specific synthesis of high density fuels by examining the significant influence of the substrate structure on the Diels–Alder reaction. When preparing polycyclic structures through Diels–Alder reactions of furan derivatives, it is advisible to consider monosubstituted furan derivatives first due to their high electron density and suitable steric resistance. The insights gleaned from this study provide substantial guidance for selecting suitable feedstocks for fuel synthesis, further contributing to sustainable energy solutions.
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Materials Science & Engineering C-Materials for Biological Applications
·
2019
·
IF 4.959
Ziyang He,Ruming Jiang,Wei Long,Hongye Huang,Meiying Liu,Junyu Chen,Fengjie Deng,Naigen Zhou,Xiaoyong Zhang,Yen Wei
Carbon nanotubes (CNTs) are a novel type of one-dimensional carbon nanomaterials that have been widely utilized for biomedical applications such as drug delivery, cancer photothermal treatment owing to their high surface area and unique interaction with cell membranes. However, their biomedical applications are still impeded by some drawbacks, including poor water dispersibility, lack of functional groups and toxicity. Therefore, surface modification of CNTs to overcome these issues should be importance and of great interest. In this work, we reported for the first time that CNTs could be surface modification through the combination of Diels-Alder (D-A) reaction and redox polymerization, this strategy shows the advantages of mild reaction conditions, water tolerance, low temperature and hydroxyl-surfaced initiator. In this modification procedure, the hydroxyl groups were introduced on the surface of CNTs through the D-A reaction that was adopted for grafting the copolymers, which were initiated by the Ce(IV)/HNO 3 redox system using the hydrophilic and biocompatible poly(ethylene glycol) methyl ether methacrylate (PEGMA) and carboxyl-rich acrylic acid (AA) as monomers. The final CNTs-OH-PAA@PEGMA composites were characterized by a series of characterization techniques. The drug loading and release results suggested that anticancer agent cis‑platinum (CDDP) could be loaded on CNTs-OH-PAA@PEGMA composites through coordination with carboxyl groups and drug release behavior could be controlled by pH. More importantly, the cell viability results clearly demonstrated that CNTs-OH-PAA@PEGMA composites displayed low toxicity and the drug could be transported in cells and still maintain their therapeutic effects.
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高影响因子
FUEL
·
2025
·
IF 7.5
Yuhang Fang,Menglong Niu,Yue Ji,Yongli Yan,Ben Niu,Xiaohua Chai,Baoqi Ma
This study aimed to enhance the combustibility of coal tar (CT) through a 2,5–dimethylfuran (DMF)-mediated ring enlargement modification, elucidate the reaction mechanism, and validate the industrial potential of modified products as high-density fuels. Catalytic reactions between DMF and CT (using AlCl 3 as the catalyst) were conducted. The modified products were characterized for chemical composition, pyrolysis behavior, and optical properties via GC–MS, TG-DTG/DSC, and UV/PL techniques. Fuel performance was evaluated through hydrogenation experiments, while reaction pathways were analyzed using Gaussian-based density functional theory (DFT) calculations to uncover mechanistic insights. Post-modification, the content of tricyclic and higher aromatic hydrocarbons (TAHs) increased significantly (20 %), with a 75 % reduction in weight loss during Stage I pyrolysis and a distinct endothermic trend in Stage III (attributed to C-O bond cleavage). UV/PL analysis revealed a 200 nm redshift in absorption peaks and a 50 nm delay in fluorescence excitation peaks, indicating increased aromatic ring numbers. Hydrogenation improved product density by 10 % (reaching 0.96 g/mL) and calorific value to 42.0 MJ/kg, confirming its superior performance as a high-density fuel. This work proposed, for the first time, a DMF-mediated ring enlargement strategy to directionally modify CT molecular structures, significantly enhancing combustibility and energy density. Experimental and DFT results systematically revealed the synergistic Diels-Alder (DA) and Friedel-Crafts (FC) alkylation mechanisms between DMF and CT, offering novel insights for high-value utilization of coal tar. The technology also held promise for applications in CT separation and pharmaceutical intermediate synthesis, demonstrating critical industrial relevance.
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JOURNAL OF BIOACTIVE AND COMPATIBLE POLYMERS
·
2017
·
IF 1.31
Dongming Xing,Lie Ma,Changyou Gao
In order to improve neurite outgrowth on the in situ formed hyaluronic acid–based hydrogel, furan and methacrylate groups were grafted on hyaluronic acid successively. Furthermore, a laminin-derived peptide CQAASIKVAV was covalently immobilized via the Michael addition. The furan- and peptide-modified hyaluronic acid was then cross-linked in situ by mixing with bismaleimide poly(ethylene glycol) at 37 °C to obtain a bioactive hyaluronic acid–based hydrogel. The hyaluronic acid derivatives were characterized by 1H NMR and Fourier transform infrared spectroscopy. The gelation, swelling, and mechanical property of the hydrogels were analyzed. The modulus of the hydrogel could be tuned by changing furan substitution degree, while the peptide concentration could be changed by the ratio of furan- and peptide-modified hyaluronic acid with hyaluronic acid–furan. In vitro culture of PC12 cells showed that the longest neurite outgrowth appeared on the hyaluronic acid–poly(ethylene glycol) hydrogel with the highest peptide content (the substitution degree of peptide in furan- and peptide-modified hyaluronic acid was 23 %) and a lower threshold modulus of 4.5 kPa. The furan and methacrylate-functionalized hyaluronic acid provides a versatile platform for diverse functionalization and can be used for modulation of other cell behaviors as well.
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POLYMER
·
2025
·
IF 4.5
Bo Zhu,Xu Sun,Yu Feng,Ji Liu,Xinyu Tao,Bo Yang
A microcapsule/XLPE composite material based on reversible Diels-Alder(DA) reaction was designed to solve the problem of electro-hydro hybrid tree aging in cross-linked polyethylene (XLPE) cables during long-term operation. Light-water dual-responsive microcapsules were prepared by in-situ polymerization using hyperbranched polysiloxane containing furan functional groups and linear polysiloxane containing furan and maleimide functional groups introduced by C C covalent bond as core materials and urea-formaldehyde resin as wall materials. A series of composites was prepared by regulating the doping concentration of microcapsules, and their insulation properties were tested. The effect of the doping content of microcapsules on the properties of materials was analyzed, and the multiple self-healing mechanism of microcapsule/XLPE composite was revealed. The results show that when the microcapsule doping concentration is 1 wt%, the composite material can self-heal while maintaining the intrinsic insulation performance of XLPE. Under the condition of thermal triggering, the dynamic reconstruction of the reversible bond enables the material to achieve dual repair of water tree and electrical tree damage, and maintains more than 80 % of the insulation performance after three times of damage-repair, which provides a new strategy for the intelligent design and life extension of high voltage cable insulation materials.
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MOLECULES
·
2026
·Vol. 31
·期 10
·1574
·
IF 5.1
Xiang Cui,Xiu-Cheng Zhu,Shu-Qi Yao,Rui Wang,Yun-Xia Zhang,Jin Li,Biao Wang,Yan-Ru Deng,Chang-Jing Wu
Alzheimer’s disease (AD) is a common neurodegenerative disorder linked to cholinergic dysfunction, with butyrylcholinesterase (BChE) being a key therapeutic target for moderate–severe AD. Cortex Mori Radicis, a traditional Chinese medicinal herb, is rich in Diels–Alder adducts with potential neuroprotective effects; here, eighteen Diels–Alder adducts (four new: morusalbanol B–E,1–4) were isolated and identified from its 80% ethanol extract. Their cholinesterase inhibitory activities were assessed via Ellman’s method, with enzyme kinetics and molecular docking performed for active compounds. Most compounds showed selective BChE inhibition, with kuwanon X (14) being the most potent (IC50= 2.3 μM). morusalbanol B (1), cathayanon A (8), and kuwanon G (12) acted as noncompetitive inhibitors, while Morusalbanol C (2) and kuwanon X (14) were mixed competitive inhibitors. Molecular docking suggested that potent inhibitors occupied the BChE active pocket via hydrogen bonds, π-π stacking, and hydrophobic interactions with Trp82, His438, and Phe329. MD simulations and MM-GBSA binding free energy analysis further verified that all three representative complexes (1,8, and14) achieved favorable thermodynamic and structural stability, with binding driven primarily by van der Waals forces. Residue decomposition revealed that Trp82 and Phe329 served as core binding hotspots for all tested inhibitors. Structure–activity analysis indicated that a cis-trans methylcyclohexene configuration, shorter aliphatic ester chains, and more prenyl groups enhanced BChE inhibition. This study provides new lead compounds and a systematic molecular mechanism basis for developing novel anti-AD BChE inhibitors from natural products.
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COMPOSITES PART B-ENGINEERING
·
2022
·
IF 11.322
Lei Zhang,Zhi Li,Qing-Qing Bi,Lin-Yun Jiang,Xiao-Die Zhang,En Tang,Xue-Meng Cao,Hong-Fang Li,Jose Hobson,De-Yi Wang
The synchronized improvement of strength , toughness and fire suppression poses to be a critical trade-off issue towards high-performance epoxy resin. Aiming to impart epoxy with balanced multifunctional improvement, the Schiff base-derived bio-based phosphaphenanthrene small-molecule reinforcer towards in-situ constructed Diels-Alder network within existing 3D network was proposed. The incorporation of 3.5 wt% reinforcer (CQ-DOPO) concurrently enhanced the tensile and impact strength of epoxy by 26.6% and 48.4% without visible deterioration of transparency. The increment of glass transition temperature by 14 °C via dynamic mechanical analysis was observed. The underpinning experimental and simulation investigation verified the proof of concept of in-situ formed Diels-Alder sacrificing network towards higher crosslinking density and strong-weak dual network. Raman spectra witnessed the breaking of sacrificing bond during fracture. Moreover, 3.5 wt% CQ-DOPO with an ultralow phosphorous loading of 0.245 wt% enabled to impart epoxy with UL-94 V-0 rating as well as limiting oxygen index of 32.0%. The multi-scale dual-phase analysis unveiled the synchronized suppression of fire reactions in vapor phase via PO· quenching as well as in condensed phase via char microstructure optimization. Hence, the rational strategy via in-situ construction of Diels-Alder sacrificing bond toward dual network exploits a novel roadmap for high-performance epoxy.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ziyu Liu,Xingyue Zhu,Yazhou Tian,Kaiyun Zhou,Jue Cheng,Junying Zhang
Polymer-based form-stable phase change materials (FPCMs) have attracted much attention due to their excellent shape stability and facileness, low-energy-consumption preparation. However, bio-based recyclable phase change energy storage materials (PCMs), crucial for reducing pollution and sustainable energy storage, have not yet been prepared. Herein, we prepared a novel bio-based recyclable PCM (DGEM-18/FA/MA/xBW), in which a novel epoxy resin (DGEM) was synthesized by using bio-based magnolol and epichlorohydrin, bio-based 2-Furanmethanamine (FA) and C36-alkylenediamines bismaleimide (MA) were used to construct a reversible crosslinked network based on epoxy-amine ring opening and Diels-Alder (D-A) reactions as the supporting frame. And 1-Octadecanethiol (ODT) and bio-based beeswax (BW) with phase change property were introduced into this supporting frame by grafting on the C=C of Magnolol via “thiol-ene” click reaction and physical blending, respectively. The D-A and rD-A reactions proceed at the temperature below 80 ℃ and above 120 °C, respectively, which provides recyclability of the crosslinked network. The ODT and beeswax provide phase change latent heat up to 119.1 J/g for the sample DGEM-18/FA/MA/1.1BW. Furthermore, taking DGEM-18/FA/MA/0.4BW as an example, its shape memory performance has been explored, as well as its potential applications in recyclable thermal management coatings. To the best of our knowledge, this is the first report on the preparation of bio-based recyclable FPCMs.
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Membranes
·
2022
·Vol. 12
·期 4
·405
·
IF 4.562
Yi Wang,Zhimin Zhou,Jiali Chen,Sixing Li,Han Zheng,Jiaxin Lu,Shuyue Wang,Jiahao Zhang,Kaiwen Lin,Ke Wang,Yuehui Wang
The hybrid composite of silver nanowires (AgNWs) and reduced graphene oxide (RGO) was synthesized in situ by an improved polyol–thermal method. The AgNWs-RGO with mass contents of 5–37 wt% was added into the thermo-reversible Diels–Alder reaction polyurethane (DA-PU) matrix with the AgNWs as the main conductor and the RGO as the auxiliary conductor to prepare self-healing composite conductive films. Further, the electrical conductivity, thermal conductivity, mechanical properties, infrared thermal response, and self-healing property of the composite film under infrared light irradiation were studied. The experimental results demonstrate that the AgNWs-RGO endows the composite film with good electrical and thermal conductivity and infrared thermal response ability, while the mechanical properties of the composite film decrease as the AgNWs-RGO mass content increases. The self-healing efficiency of the composite film is higher than that of the pure DA-PU under infrared light irradiation due to the good infrared photothermal response ability of the AgNWs-RGO. When the mass content of AgNWs-RGO in the composite film was 25 wt%, the AgNWs-RGO showed good dispersion in composite films, and the resistivity, thermal conductivity, and tensile strength of the composite film were 0.544 Ω·m, 0.3039 W·m−1·K−1, and 9.05 MPa, respectively. The infrared photothermal conversion temperature of the composite film is 158.5 °C (3450 lux for 1 min), and the infrared photothermal self-healing efficiency is 118% (3450 lux for 600 s). The AgNWs-RGO also improves the multiple self-healing ability of the composite film. The use of a high mass content of AgNWs-RGO in the composite film is beneficial in obtaining high multiple self-healing efficiencies. The first and the fifth infrared thermal self-healing efficiencies of the composite film with AgNWs-RGO of 35 wt% are 105% and 86%, respectively, and the resistivity of the composite film changes little and still maintains good conductivity.Keywords:silver nanowires;reduced graphene oxide;thermo-reversible Diels–Alder reaction polyurethane;self-healing;flexible conductive film
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