Chemical Science
·
2025
·
IF 7.4
Zihao Guan,Lulu Fu,Lu Chen,Zhiyuan Wei,Fang Liu,Yang Zhao,Zhipeng Huang,Mark G Humphrey,Chi Zhang
The long-chain ligands and weak charge-transport capacity of perovskite nanocrystal (NC) always hinder its optoelectronic applications. Our study proposes an effective strategy to unlock the optimized nonlinear optical (NLO) properties of perovskite via the aromatic ligand-exchange plus porphyrin-axial-coordination. Synthesized porphyrin-pyridine dual-modified CsPbBr3-NC hybrid material, fabricated by 4-(aminomethyl)pyridine (PyMA) and a novel star-shaped zinc-porphyrin trisubstituted triazacoronene compound (ZnPr) modifications, exhibits excellent NLO absorption performance under femtosecond (fs) laser irradiation in the visible to near-infrared range. Specifically, its nonlinear absorption coefficient is 10 times higher than that of the pristine CsPbBr3-NC and it also possesses an outstanding optical limiting (OL) capability with an OL threshold as low as 1.8 mJ cm−2. The modification of PyMA ligands reduces the trap state density on the perovskite surface and promotes the electronic coupling between the NC lattices. With the aid of PyMA coordinating with the Zn atoms in ZnPr, large-size planar porphyrins are anchored on the perovskite surface from the axial position, which may enhance the ligand protection capability and thereby significantly facilitate the charge transport between porphyrin components and perovskite NCs. The above two-step modification synergistically contributes to the prominent NLO performance. Our work affords a new viable paradigm for developing multi-field and high-performance perovskite NC photonic materials and devices.
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高影响因子
MOLECULES
·
2025
·Vol. 30
·期 4
·787
·
IF 4.6
Shuaihua Liu,Tian Yao,Donghui Xia,Quan Liu,Guanghui Tian,Yang Liu
Low-molecular-mass gelators (LMMGs) as stabilizers for gel emulsions offer numerous advantages, such as low usage, functionalizability, and insensitivity to phase ratio. Using LMMGs as stabilizers is one of the effective strategies for preparing gel emulsions. Currently, developing LMMGs and stable gel emulsion systems in a rapid and convenient manner remains a challenge. To cope with the challenge, this study aims to develop a simple and efficient gel emulsion preparation method based on LMMGs. In this study, a cholesterol-based star-shaped derivative (CSD) was designed and synthesized as an LMMG. Based on gelation experiments, a high internal phase W/O gel emulsion system (H2O/CSD-poly(oligo)-dimethylsiloxane/dichloromethane) was successfully developed and stabilized synergistically by the stabilizer (CSD) and the crosslinker (poly(oligo)-dimethylsiloxane with two olefinic bonds at its ends, D-PDMS). The results demonstrate that the synergistic interaction between CSD and D-PDMS is critical for the formation of the gel emulsion. Building on the original gel emulsion system, two novel in situ polymerizable gel emulsion systems (H2O/CSD-D-PDMS/dichloromethane-tert-butyl methacrylate and H2O/CSD-D-PDMS/dichloromethane-N-tert-butyl methacrylamide) were successfully developed by introducing suitable amphiphilic (hydrophilic/lipophilic) polymerizable monomers. This study found that changes in the amphiphilicity of the introduced monomers significantly affected the stability and microscopic morphology of the gel emulsion system. The findings indicate that constructing a hydrophilic/lipophilic balanced system via the synergistic action of stabilizers and crosslinkers in a solvent system, followed by the introduction of polymerizable monomers, is a simple and efficient method for rapidly developing novel polymerizable gel emulsions. These new polymerizable gel emulsions lay the foundation for the subsequent preparation of porous organic polymers (POPs).
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ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Hui Bai,Lei Chen
Background As the derivatives of cyclodextrin (CD), cyclodextrin polymers (CDPs) effectively increase the concentration of CD units and construct supramolecular structures with unique stereoselectivity by the structure design. CDPs have shown significant potential in chiral separation, however, the process of stereoselective interactions on chiral stationary phases (CSPs) and the specific contribution of intermolecular forces are still a challenge issue. A comprehensive understanding of the chiral recognition mechanism of CDPs will help to optimize chiral separation conditions and design new CSPs. Results The star CDP with a supermolecular structure was synthesized by grafting β-CD onto the external 6-position hydroxyl groups using β-CD as the parent nucleus. The enhanced host-guest recognition ability of CD supramolecular polymer structure provided better inclusion interaction and increased chiral recognition of the isomers. The Star-CD CSP with star CDP as a chiral ligand performed satisfactory stereoisomer separation ability with the separation factor (α) up to 2.0 for various quinoline alkaloid isomers and 1.89 for catechins. To elucidate its chiral separation mechanism, molecular docking was used to construct the three-dimensional visual models of the binding sites and the contribution of non-covalent interactions between Star-CD CSP and quinoline alkaloid isomers. In addition, the formation sites of non-covalent interactions on the CD monomers of the polymer side chains were confirmed from the actual geometric structure by analyzing the NMR chemical shift changes before and after the formation of complexes between Star-CD polymers and isomers. Combined with the mutual evidence of molecular simulation and chiral NMR, the specific recognition mechanism of selector-selectand complexes was comprehensively expounded. Significance The multi-mode CSP based on cyclodextrin supramolecular structure provides new ideas for the stereoisomeric separation of complex chiral components with multiple chiral centers in natural products. Not limited to the macroscopic performance of the chromatographic separation, molecular docking explored the theoretical model of chiral recognition from the molecular level. The chiral NMR analysis confirmed the credibility of the model from the geometry structure, and then the recognition mechanism of multi-mode CSP was fully elaborated combining the above three aspects.
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高影响因子
CHIRALITY
·
2021
·Vol. 34
·期 1
·61-69
·
IF 2.437
Hui Zou,Wen-Quan Liang,Qi-Liang Wu,Li Zhou,Xiao-Hua Hou,Na Liu,Zong-Quan Wu
Helical polymers present some interesting and distinctive properties, and one of the most distinguished applications of them is the chiral recognition and resolution of enantiomers. In this work, star-shaped hybrid helical poly (phenyl isocyanide) (PPI) with polyhedral oligomeric silsesquioxanes (POSS) as the core was designed and synthesized by “grafting to” strategy. The homoarm star-shaped hybrid POSS-(PPI) 8 was first obtained by the click reaction between azide-modified POSS (POSS-(N 3 ) 8 ) and alkynyl-modified PPI (PPI-Alkynyl). The hybrid POSS-(PPI) 8 was with predominated left-handed helical conformation and exhibited excellent ability in the enantioselective crystallization of racemic compounds. In the meantime, heteroarm star-shaped hybrid (PEG) 4 -POSS-(PPI) 4 was prepared by the click reaction of POSS-(N 3 ) 8 with PPI-Alkynyl and alkynyl-modified poly (ethylene glycol) (PEG-Alkynyl). The hybrid (PEG) 4 -POSS-(PPI) 4 was amphiphilic, and it could self-assemble to form spherical micelles in aqueous solutions.
研究领域:
高分子化学
·
材料科学
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高影响因子
International Review of Financial Analysis
·
2024
·
IF 7.5
Shengpeng Zhang,Yaokuang Li,Yu He,Ruixin Liang
In this study, we investigate whether vocal cues expressed by management in IPO online roadshows in the SSE STAR Market play an information role. Using deep learning techniques, we classify the emotional tendencies of vocal cues in IPO online roadshows and construct quantitative proxy variables. After a series of empirical analyses, we find that vocal emotions are positively associated with first-day stock returns after IPO. In addition, we find that vocal emotions have predictive power for future operating performance after IPO. Our findings still hold after a series of robustness checks. Through additional analyses, we provide evidence that information content in the prospectus and investor sentiment play moderating and mediating roles, respectively, in the relationship between vocal emotions and the first-day stock returns after IPO. Moreover, we find that the vocal emotions expressed in the presentation section and the management tone in the Q&A section develop synergistic effects. Finally, we find that the information role played by vocal emotions exhibits timeliness. Our findings elucidate the information role of vocal cues and highlight the importance of IPO online roadshows in the SSE STAR Market.
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高影响因子
JOURNAL OF MATERIALS CHEMISTRY
·
2011
·Vol. 21
·期 28
·10390-10398
·
IF 5.101
Kunmin Yang,Hui Liang,Jiang Lu
A well-defined multifunctional star polymer consisting of reactive and thermoresponsive poly(N-isopropylacrylamide-co-acrolein) arms and an aluminum tris(8-hydroxyquinoline) (Alq3)-bearing fluorescently labeled core was synthesized via reversible addition-fragmentation chain transfer (RAFT) polymerization using the “arm-first” method. Acrolein, a commercially available aldehyde-bearing monomer, was copolymerized with N-isopropylacrylamide (NIPAM) via RAFT technique in a controlled way to give well-defined linear trithiocarbonate terminated poly(NIPAM-co-acrolein) macro-RAFT agent. The preformed linear macro-RAFT agent was then cross-linked by a tri-vinyl Alq3-containing cross-linker (Alq3 cross-linker) in conjunction with N,N′-methylenebisacrylamide to give the desired reactive, thermoresponsive, and fluorescently labeled star polymer. The resultant star polymer exhibits a lower critical solution temperature at ∼29.8 °C in water, and displays intense greenish-yellow fluorescence with maximum emission peak around 520 nm in both organic solvent (i.e., THF) and water. Moreover, the highly reactive aldehyde functions in the arms of the star polymer could provide the key intermediates to conjugate biomolecules, and the conjugation with an aminooxy-functionalized BSA model protein was also demonstrated as an example of how the novel star polymer can be utilized to conjugate bioactive molecules, constructing fluorescently labeled “smart” polymer-protein conjugates.
研究领域:
高分子化学
·
生物材料
·
生物化学
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高影响因子
Materials Science & Engineering C-Materials for Biological Applications
·
2017
·
IF 4.164
Fangyuan Guo,Dongxue Huang,Wei Zhang,Qinying Yan,Qingliang Yang,Yan Yang,Hanbing Li,Junxian Yun,Weiyong Hong,Gensheng Yang
Elastomers are largely developed for biomedical applications; however, little is reported on them although they are an effective and controllable delivery system for proteins. In the present study, we investigated the pharmacokinetics, biosecurity, and hypoglycemic effect of an insulin-loaded elastomer formulation in diabetic rats. Cylindrical insulin-loaded elastomers were fabricated using a UV cross-linking process based on methyl-acrylic- star -poly(ε-caprolactone- co -D,L-lactide) cyclic ester and methyl-bi-acrylic-poly(ε-caprolactone-b-polyethylene glycol-b-ε-caprolactone) (CLPEGCLMA). The encapsulated insulin was well protected during the formulation. An in vitro pharmacokinetic study revealed that the rate of insulin release from the elastomers was affected by the hydrophilicity/hydrophobicity of the system and controlled by the CLPEGCLMA (hydrophilic prepolymer) composition. It was observed that insulin release followed the Higuchi model. In addition, the more hydrophilic elastomers showed higher degradation rates in vivo . Furthermore, in the pharmacodynamic study, all the elastomers, except those that contained star -poly(ε-caprolactone- co -D,L-lactide) (number-average molecular weight, Mn), polyethylene glycol (PEG) (kMn), ε-caprolactone/PEG (mol/mol), and CLPEGCLMA (weight, %) at a ratio of 3432:10:20:30, respectively, decreased blood glucose concentration and maintained it at a stable level. It was observed that the hypoglycemic effect of the drug-loaded elastomers was directly proportional to the rate of in vitro insulin release; however, emaciation was not observed. Moreover, elastomers play a positive role in biosecurity. Therefore, the elastomers might be effective carriers for the delivery of peptide drugs in the form of implants.
研究领域:
生物医学工程
·
药物学
·
材料科学
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高影响因子
MACROMOLECULAR BIOSCIENCE
·
2017
·Vol. 17
·期 7
·1600522
·
IF 3.238
Li Zhang,Dongjian Shi,Chunling Shi,Liangliang Dong,Xiaojie Li,Mingqing Chen
Novel biodegradable polymers with specific properties, structures, and tailorable designs or modifications are in great demand. Poly(phosphoester)s with good biocompatibility and degradability, as well as other adjustable properties have been studied widely because of their potential in biomedical applications. To meet more versatile and diverse biomedical applications, a novel multiarm star-shaped phosphorester triblock copolymer poly(amido amine)- block -poly(2-butynyl phospholane)- block -poly(2-methoxy phospholane) (PAMAM-PBYP-PMP) is synthesized via organo-catalyzed sequential ring-opening polymerization. Supramolecular micelles with good architectural stability are self-assembled into uniform spherical morphology in aqueous solution. Doxorubicin (DOX) can be encapsulated into the micelles with efficient loading capacity. A slow and sustained release in the environment of simulated intracellular lysosome (pH 5.0 with phosphodiesterase I) is observed. In addition, the copolymers and DOX-loaded supramolecular micelles exhibit low cell-toxicity and excellent anticancer activity toward HeLa cells. As a consequence, this multiarm star-shaped PAMAM-PBYP-PMP has great potential in drug delivery system for tumor treatment.
研究领域:
材料科学
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生物医学工程
·
药学
·
纳米技术
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高影响因子
RSC Advances
·
2017
·Vol. 7
·期 14
·8484-8490
·
IF 3.108
Hui Xue,Lun Peng,Yishi Dong,Yuqing Zheng,Yafei Luan,Xiang Hu,Gaojian Chen,Hong Chen
In this paper, novel star glycopolymers were synthesized via Cu(0)-mediated radical polymerisation at ambient temperature. The reaction was fast with little star–star coupling. Moreover, star glycopolymers can be obtained without removing oxygen from the polymerisation mixture. The effects of solvent and the ratio of initiator/catalyst/ligand on polymerisation were investigated, and the optimal conditions for the synthesis of star glycopolymer were determined. In addition, the binding ability between synthesised glycopolymers and concanavalin A (ConA) was studied using a turbidity test and quartz crystal microbalance-dissipation (QCM-D). Compared with linear glycopolymers, star glycopolymers showed higher binding ability to specific lectins and the strongest binding was obtained when the molecular weight was medium.
研究领域:
高分子化学
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材料科学
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生物化学
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高影响因子
Polymer Chemistry
·
2017
·Vol. 8
·期 27
·4043-4051
·
IF 5.375
Wenhua Yang,Changmin Yu,Chunxian Wu,Shao Q. Yao,Shuizhu Wu
MicroRNAs (miRNAs) are small regulatory noncoding RNAs that control a variety of biological processes. The regulation of many endogenous miRNAs is tightly associated with various diseases. Thus, the design of miRNA delivery systems with minimal endolysosomal trapping, efficient delivery and controlled miRNA release is urgently needed. Herein, we have developed a new star polymer which consists of a β-cyclodextrin (βCD) core and multiple cell-penetrating poly(disulfide) (CPD) arms. By subsequently loading the system with miRNAs and small molecule drugs, we have successfully proven that this novel drug delivery platform could efficiently enter mammalian cells (<2 h) without apparent endolysosomal trapping. The global Pearson's R value was calculated to be 0.31 between our complex and endolysosome, which is far below the threshold of >0.5 required for correlation. In addition, the GSH-triggered degradation of CPD arms and the subsequent intracellular release of miR-203 and CPT, as well as the combination therapeutic effects have been successfully demonstrated. In this way, we show that this novel platform could be used in future to minimize potential cytotoxicity encountered by many existing cationic branched polymer systems in miRNA delivery. Our results provide important starting points for using CPD-based polymers to design personalized delivery platforms.
研究领域:
药学
·
生物技术
·
分子生物学
·
药物递送系统
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高影响因子
Journal of Macromolecular Science Part A-Pure and Applied Chemistry
·
2009
·
IF 0.72
Shenwen Fang,Ming Duan,Chunyong Jiang,Liehui Zhang,Jian Zhang
Water-soluble thioxanthone-terminated poly(ethylene imine) (PEI 600, PEI 1800, PEI 3000 and PEI 10000; 600, 1800, 3000 and 10000 are the weight-average molecular weights of the above PEIs, respectively). Macrophotoinitiators were synthesized by introducing a certain amount of thioxanthone (TX) moieties into the periphery of PEI, and the products were confirmed by 1H-NMR, FT-IR, and elemental analysis. Star polyacrylamides (PAMs) were prepared using the obtained macrophotoinitiator as a core via photopolymerization. The effect of the molecular weight of the macrophotoinitiator on photoinitiation efficiency of the resulting polymers was investigated. The result shows that the choice of the macrophotoimitator has no influence on the rate of polymerization. In addition, three plots of characteristic properties with the star polymer were studied to confirm the existence of arms in the resulting star PAM.
研究领域:
高分子化学
·
光化学
·
材料科学
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高影响因子
EUROPEAN POLYMER JOURNAL
·
2020
·
IF 3.862
Mi Zhou,Feng Ling,Jie Li
We now report a star-shaped supramolecular copolymer for diagnosis and treatment by chelated with Gd 3+ ion as magnetic resonance imaging (MRI) contrast agent and drug-carried for controlling release agent. The copolymer is prepared by the host-guest inclusion complexation between the host polymer polycaprolactone-β-cyclodextrin (4sPCL-CD) and the guest polymer adamantylamine-poly-L-lactic-block-poly(N-isopropylacrylamide-co-2-hydroxyethylmethacrylate-diethylenetriamine penta acetic acid) (AD-PLLA- b -P(NIPAM- co -HEMA-DTPA)) and can self-assemble into spherical micelles in aqueous solution. By adding 2-adamantylamine hydrochloride (AD-NH 2 ), the supramolecular copolymer can be disassembled to the host and guest polymers and its molecular weight will be decreased. When the polymeric micelles are chelated with Gd 3+ ion, they exhibit T 1 relaxivity as a kind of contrast agent for MRI. This contrast agent can maintain a large molecular size to stay in vivo and also can reduce its molecular size quickly and metabolize rapidly from the body by disassembled. Also, as the copolymer carries drugs, it displays burst release and thermal-response release behaviors, due to its dis-assembly and thermal-response PNIPAM chain respectively. Thus, the supramolecular copolymer from the host-guest inclusion complexation is expected to realize diagnosis and treatment feature for clinic.
研究领域:
材料科学
·
医学影像
·
药物递送
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高影响因子