CHEMISTRY-A EUROPEAN JOURNAL
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2024
·
IF 3.9
Dandan Li,Wenrong Zhao,Gang Li,Yan Xu,Liang Xu,Bo Tang
Graphical Two novel star-shaped fluorophores named PDI−S and PDI−Se are constructed by S/Se-fused perylene diimides (PDIs) connected with bicarbazole core. Particularly, PDI−S presents excellent two-photon absorption cross-action (δ TPA ) of 3775 GM excited with 800 nm light, which is the highest value based on PDIs motif in the NIR−I region (700–900 nm). Two-photon absorption (TPA) has attracted growing attention over recent years owing to the wide range of applications in organic nonlinear optical (NLO) materials. The quantitative sensitivity of a two-photon molecular entity is determined by its TPA cross-section (δ TPA ). Perylene diimides (PDIs) are excellent n-type organic semiconductor materials demonstrating distinguished thermal, optical, and chemical stability. Nonetheless, PDIs-based scaffolds exhibit poor δ TPA in the NIR−I region (700–900 nm) due to the lack of suitable molecular design. Here, two novel star-shaped PDIs fluorophores, namely PDI−S and PDI−Se, were constructed by four periphery S/Se-fused PDIs connected with bicarbazole core. PDI−S manifested excellent δ TPA of 3775 GM, which are among the highest values reported for PDIs excited in the NIR−I region.
研究领域:
有机化学
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材料科学
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Journal of Macromolecular Science Part A-Pure and Applied Chemistry
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2014
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IF 0.74
Yan Xue,Dafu Wei,Anna Zheng,Yong Guan,Huining Xiao
Cationic star polymers as drug/gene carriers have attracted increasing attention. Herein, environmental sensitivities and star-shaped architecture were combined into a well-defined gene carrier system, and further amphiphilic modification was conducted. The thermo- and pH-sensitive behaviors of poly[N,N-(dimethyl amino)ethyl methacrylate] (PDMAEMA) star polymers before and after amphiphilic modification in aqueous solutions were investigated. The observed lower critical solution temperature (LCST) increased with increasing arm length due to the increase of hydrophilicity. A significant decrease of the LCSTs with increasing pH and ionic-strength of the solution was found. The incorporation of MMA and BA lipophilic moieties decreased the LCST of the cationic star polymer due to enhanced hydrophobic interaction. As a potential gene carrier, the performance of star polymers on binding DNA was primarily evaluated via particle size, zeta potential, and gel retardation measurements. All the complexes formed stable small particles with diameter of 100∼150 nm at N/P ratio higher than 3.0. The electrostatic screening effect and facilitation for the interaction of complexes with cell membrane induced by the incorporation of lipophilic units were expected to enhance the gene transfection efficiency.
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MACROMOLECULES
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2026
·
IF 5.7
Kangle Zhou,Junhong Guo,Junchen Wu,Kun He,Suli Chen,Tianxi Liu
Poly(ethylene oxide) (PEO)-based solid electrolytes are pivotal for enabling high-safety and high-energy-density all-solid-state lithium metal batteries (ASSLMBs) yet remain fundamentally constrained by the inherent trade-off between ionic conductivity and mechanical robustness. Herein, we report a supramolecularly expanded polymer electrolyte engineered via a star boron-cored poly(ethylene glycol) (BPEG) macromolecule. The BPEG architecture incorporates a Lewis acidic boron core that promotes salt dissociation through anion-trapping, along with three flexible PEG arms that are intrinsically ion-conductive and structurally homologous to the PEO matrix. Critically, these PEG arms mediate the formation of a dynamic multiscale hydrogen-bond network between the PEO chains. This unique architecture, which disrupts PEO crystallization to unlock segmental motion, operates on a sequential relaxation mechanism: labile weak hydrogen bonds dissociate preferentially to facilitate Li+ transport, while robust strong hydrogen bonds persist to maintain mechanical integrity. Such design yields a robust yet adaptive supramolecular network that concurrently establishes continuous ion-conduction pathways and enhances structural robustness. As a result, the SEPE demonstrates high ionic conductivity, improved mechanical strength, and stable interfacial compatibility with lithium metal, enabling highly stable Li plating/stripping and delivering excellent performances in high-loading practical ASSLMBs. This work introduces a feasible multiscale relaxation supramolecular strategy for high-performance polymer electrolytes.
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EUROPEAN POLYMER JOURNAL
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2021
·
IF 4.598
Qingfu Ban,Yan Li,Yusheng Qin,Yaochen Zheng,Jie Kong
Hyperbranched star copolymers are important soft materials that have been employed for aqueous self-assembly and bioapplication, but their one-pot one-batch synthesis strategy and relevant topology are rarely discussed. In this contribution, we produce hyperbranched star poly(vinyl ether ester)s (mPEG- hb -PVEEs) amphiphiles with multimodal molecular weight distribution via one-pot one-batch Am+Bn+C1 (m ≥ 2, n ≥ 3) step-growth polymerization. Based on the topological analysis of these hyperbranched star copolymers, a convenient expression of the number ratio of monomeric structural units (N A /N B ) is deduced to describe the cyclic defect of intramolecular cyclization only by using proton nuclear magnetic resonance spectroscopy. The introduction of long-chain terminators and the change in the molar feed ratio of A 2 :B 3 :C 1 considerably affect the N A /N B so as to give rise to increased influence of number of macromolecules and decreased influence of intramolecular cyclization, which are then responsible for an aqueous self-assembly behavior of mPEG- hb -PVEEs amphiphiles. Overall, this study opens new possibilities for the precise description of intramolecular cyclization and controllable synthesis of hyperbranched star copolymers via one-pot Am+Bn+C1 step-growth polymerization.
研究领域:
高分子科学
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材料科学
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化学工程
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生物技术
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ELECTROCHIMICA ACTA
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2019
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IF 5.383
Ning Zhou,Yufeng Wang,Yang Zhou,Jinyou Shen,Yong Zhou,Yong Yang
Star-shaped polymeric ionic liquids (PIL-3 and PIL-4) based on poly(2-(dimethyl-ethyl-amino)ethyl methacrylate) bis(trifluoromethylsulfonyl)imide (P(EtDMAEMA-TFSI)) with three-arm and four-arm architectures were prepared through atom transfer radical polymerization (ATRP) and ion exchange. Subsequently, gel polymer electrolytes (GPEs) comprising PIL host, N,N-diethyl-N-methyl-N-(2-methoxyethyl)ammonium bis(trifluoromethylsulfonyl)imide (DEME-TFSI) ionic liquid (IL) plasticizer with the same anion unit and LiTFSI salt were obtained. Compared with the linear PIL possessing the same elements, the increase of branches for PIL decreases the crystallity and glass transition temperature (T g ) of the corresponding GPEs. Accordingly, the ionic conductivity , electrochemical window and ion transport number of three-arm and four-arm PILs based GPEs (PIL-GPE-3 and PIL-GPE-4) are obviously superior to the linear contrastive sample. Among lithium metal batteries assembled by linear, three-arm and four-arm PILs based GPEs, Li/PIL-GPE-4/LiFePO 4 presents the best performance. The specific discharge capacity attains 151 mAh g −1 at 0.1 C, the capacity retention ratio achieves 93.6% after 100 cycles at 60 °C, and the coulombic efficiency is around 99%. The outstanding compatibility between PIL-4 and IL and the resulted interfacial stability between PIL-GPE-4 and electrodes both contribute to the excellent performance.
研究领域:
材料科学
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电化学
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能源存储
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Polymer Chemistry
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2012
·Vol. 3
·期 9
·2656-2664
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IF 5.321
Chunlei Zhang,Miao Miao,Xueteng Cao,Zesheng An
The arm-first approach is well accepted for the synthesis of core cross-linked star (CCS) polymers, which typically involves two separate steps, i.e., the initial synthesis and purification of the arm polymers followed by a second step synthesis of CCS. We report here a one-pot approach for the RAFT synthesis of a well-defined CCS in water without the separation and purification of the arm polymers. This novel approach consists of a homogeneous polymerization step to prepare the arm polymer, polyPEGMA, and a heterogeneous polymerization step to assemble the arm polymers into CCS polymers. Various parameters affecting the formation of the CCS were studied, including the type of cross-linker, spacing monomer, arm polymer concentration and arm polymer molecular weight. Cross-linkers of longer length provided the flexibility required to form high-quality CCS polymers. The use of spacing monomers in conjugation with cross-linkers reduced the stress during cross-linking and also provided enhanced driving force to produce well-defined CCS polymers. High-quality CCS polymers were prepared at relatively high polymer concentration (≥10%). The higher molecular weight arm polymer exhibited increased steric hindrance for CCS formation. Overall, this one-pot approach is highly efficient, environmentally benign and amenable to a variety of reaction conditions.
研究领域:
高分子化学
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材料科学
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高影响因子
COMPARATIVE BIOCHEMISTRY AND PHYSIOLOGY C-TOXICOLOGY & PHARMACOLOGY
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2022
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IF 4.52
Long Zhu,Mingrong Wang,Shuo Fu,Kaiqi Li,Jialin Liu,Zaizhao Wang
Bisphenol A (BPA) is a widely used endocrine disruptor , which has attracted much attention due to its harmful effects on male reproduction. To investigate the interference of BPA on steroid synthesis in males, male rare minnows ( Gobiocypris rarus ) were exposed to 15 μg L −1 BPA for 7, 14 and 21 d. Meanwhile, a positive control group was performed with 25 ng L −1 17α-ethynyl estradiol (EE2). Results showed that BPA exposure induced lower testosterone (T) levels, while affecting the transcripts of steroidogenic gene StAR . Moreover, BPA induced abnormal germ cells proliferation in the testis in rare minnow. Transcriptome analysis showed that 354 transcripts significantly differentially expressed after BPA exposure for 14 d, several of them were enriched in the signaling pathways of cell cycle process, PPAR signaling pathway, the steroid synthesis pathway and estrogen signaling pathway. BPA significantly increased estrogen receptor (ER) levels and induced abnormal protein levels of PPARγ. BPA disrupted the StAR expression by interfering ER enrichments within StAR 5′ flanking region . Additionally, our study also revealed that BPA and EE2 might have different mechanisms for interfering with steroid hormone levels and germ cells proliferation in the testis.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2015
·Vol. 132
·期 31
·
IF 1.768
Xiongfa Yang,Cheng Cao,Zhonghong Chen,Jia Liu,Alan R. Bassindale,Guoqiao Lai
Combination of the organic–inorganic hybrid such as silsesquioxane with ε-caprolactone will lead to materials expected to be environmentally friendly and applicable to biomedical usages. A ladder-like poly(phenyl silsesquioxane) based hybrid star-shaped copolymer of ε-caprolactone was prepared by ring opening polymerization of ε-caprolactone catalyzed by Sn(Oct) 2 with hydroxyl terminated ladder-like poly(phenyl silsesquioxane) as initiator. The copolymers were characterized by proton nuclear magnetic resonance ( 1 H-NMR), silicon nuclear magnetic resonance ( 29 Si-NMR), Fourier-transform infrared spectrometer (FT-IR), size exclusion chromatography (SEC), thermo gravimetric analysis (TGA), and differential scanning calorimetry (DSC) in detail. Furthermore, the enzymatic degradation property of the copolymers was also investigated. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132 , 42335.
研究领域:
材料科学
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生物医学工程
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BIOMACROMOLECULES
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2016
·
IF 5.583
Mengying Hu,Yurun Shen,Lu Zhang,Liyan Qiu
To date, improving oral bioavailability of water-soluble drugs with poor membrane permeability is still challenging. An example of this includes doxorubicin hydrochloride (DOX·HCl), a widely used chemotherapeutic. We therefore developed a novel DOX·HCl-loaded polymersome (Ps-DOX·HCl) self-assembled by amphiphilic β-cyclodextrin-centered triarm star polymer (mPEG2k-PLA3k)3-CD with the considerable drug loading capability. Using Madin-Darby canine kidney (MDCK) cells trans-well models, it was found that the cellular uptake and absorptive transport of DOX·HCl was significantly increased and the efflux was attenuated when delivered through polymersomes than free drugs. This phenomenon was further verified in mechanistic studies, which was attributed to the change in membrane transport pathway from paracellular route (free DOX·HCl) to active transcellular transport (drug-loaded polymersomes). Moreover, in vivo pharmacokinetic studies in mice demonstrated a significant increase in the oral bioavailability of Ps-DOX·HCl compared with free DOX·HCl (7.32-fold), as well as extended half-life (8.22-fold). This resulted in a substantial anticancer efficacy against mouse sarcoma 180 (S180) tumor in vivo. The cardiotoxicity, which is intrinsically induced by DOX·HCl, and toxicity toward gastrointestinal tissues were avoided according to histological studies. These findings indicate that (mPEG2k-PLA3k)3-CD copolymer displays great potential as a vehicle for the effective oral delivery of water-soluble drugs with low permeability.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Peiyi Liu,Bin Wang,Yu Chen
Flexible poly(vinyl chloride) (PVC) plastics have been widely used in medical devices, but the preparation of antibiofouling flexible PVC materials that can maintain their antibiofouling performance when suffering deformation is still a challenge. In this work, we synthesized a series of amphiphilic star-shaped three-arm block copolymers SPCL-b-PSB, consisting of hydrophobic inner blocks poly(ε-caprolactone) (PCL) and hydrophilic outer blocks poly(methacryloxyethyl sulfobetaine) (PSB). Then, flexible PVC films were prepared by blending SPCL-b-PSB with PVC and plasticizer. Benefiting from the specific star-shaped topological structure of SPCL-b-PSB, hydrophilic PSB blocks of the copolymer could efficiently migrate to the surface of the film via annealing treatment, which give the film surface excellent hydrophilicity, while the latch-like entanglements between hydrophobic PCL blocks and PVC give the hydrophilic surface excellent stability. Antibiofouling properties of the blended films were investigated. The optimized blended film could reduce ∼94% of bovine serum albumin adsorption, ∼ 87% of lysozyme adsorption, and ∼89% of platelet adhesion and resist bacterial adhesion effectively. What is more, the blended films could maintain their antibiofouling performance when suffering stretching, rubbing, or bending. More than 86% of bovine serum albumin adsorption could be reduced, even when the film was stretched by 50%. This work provides a new strategy for the preparation of durable antibiofouling flexible plastics.
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POLYMER
·
2018
·
IF 3.483
Qijing Chen,Fei Han,Chao Lin,Xuejun Wen,Peng Zhao
The aim of this study is to synthesize well-defined bioreducible core crosslinked star (CCS) polymers via heterogeneous reversible addition-fragmentation transfer (RAFT) polymerization in aqueous ethanol solutions. To this end, water-soluble linear arm polymers, poly (poly (ethylene glycol) methyl ether methacrylate) (PPEGMA), poly (2-(dimethylamino)ethyl methacrylate) (PDMAEMA) and poly ( N , N -dimethylacrylamide) (PDMA), were prepared respectively. Next, heterogenous RAFT polymerization of the polymers with N , N ′-bis(acryloyl)cystamine (BAC) as a crosslinker was systemically investigated in an aqueous ethanol solvent. It was found that these bioreducible CCS polymers with crosslinked BAC core could be prepared successfully depending on polymerization parameters. The formation of PPEGMA-based CCS polymers was affected by water volume fraction ( V w ) of water-ethanol solution, reaction time, arm polymer concentration, and spacing monomer . Besides, at an optimal V w of 80% ( i . e . the molar concentration of water is 44.44 M) and arm polymer concentration of 10% (w/v), PPEGMA-based CCS polymers at >90% yield could be achieved within 1 h. By the same V w and reaction time, PDMAEMA- and PDMA-based CCS polymers could also be prepared with high yield (>75%). The mechanism underlying the formation of the CCS polymers was ascribed to enhanced driving force of polymerization-induced self-assembly at an optimal V w . These CCS polymers were degradable in thiol-containing dithiothreitol, suggesting their potential application for drug release in a reductive intracellular environment.
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JOURNAL OF CHROMATOGRAPHY A
·
2018
·
IF 3.716
Yinhui Yang,Meiling Qi,Jinliang Wang
This work describes the separation performance of a star-shaped truxene-based material (denoted as EDOTT) as the stationary phase for capillary gas chromatography (GC). The EDOTT capillary column achieved the column efficiency of 5920 plates/m by n -dodecane, 4890 plates/m by naphthalene and 3960 plates/m by 1-octanol at 120 ℃. Its selectivity and retention behaviour were investigated by a number of mixtures of diverse analytes and their isomers. As a result, it showed advantageous performance for separations of apolar to polar analytes, especially phenols and alcohols, over its analogous TTT, TDT and TFT stationary phases. In addition, the EDOTT capillary column was investigated for its column loadability, repeatability and thermal stability, and was finally applied for the determination of isomer impurities in real samples. This work provides an alternative truxene-based stationary phase with high selectivity for polar analytes and demonstrates the key role of structural modification in developing a family of stationary phases with specific selectivity for targeted analytes.
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