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JOURNAL OF INCLUSION PHENOMENA AND MACROCYCLIC CHEMISTRY · 2016 ·Vol. 87 ·期 1 ·67-74 · IF 1.253

Perhydroxycucurbit[6]uril-induced self-assembly of a double-hydrophilic block copolymer in aqueous solution

Wang Zhipeng,Li Mingrui,Huang Xiaoling

We reported the preparation of the poly( N -vinyl pyrrolidone)-b-polyethylene glycol (PVP-b-PEG) double-hydrophilic block copolymer by atom transfer radical polymerization (ATRP). The PVP-b-PEG samples were characterized by nuclear magnetic resonance spectroscopy and Fourier translation infrared spectrum. By taking advantage of its exceptional binding affinity, the perhydroxycucurbit[6]uril ((HO) 12 CB[6]) was used to interact with PVP-b-PEG by hydrogen bond and constructed micelle-like core–shell aggregates with the physical cross-link PVP segments as the core and the extending PEG chains as the outer palisade. The size of aggregates was about 50–300 nm. The particle size of this type of assemblies could be controlled by the weight content of (HO) 12 CB[6]. The size distribution was broad at high concentrations. The broad size distribution at high (HO) 12 CB[6] concentration was due to the coexistence of isolated particles and clusters. These novel micelle-like core–shell aggregates could be controlled by pH value. At pH lower than 6 or pH larger than 13, hydrogen bond interactions were destroyed and the formed (HO) 12 CB[6]-induced PVP-b-PEG assemblies could be destructed.

研究领域: 高分子化学 · 纳米材料科学 · 超分子化学
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Small · 2024 ·Vol. 20 ·期 51 ·2406072 · IF 13

Long-Term Resistance to Phase Change-Induced Wetting Transition on Biphilic Armored Superhydrophobic Surfaces

Zhenda Liu,Dagui Wang,Wei Zhang,Shan Gao,Yang Shen,Zhenxu Shi,Binyang Lu,Dehui Wang,Xu Deng

Material surfaces maintaining a liquid super-repellent is crucial in fields such as anti-fouling, drag reduction, and heat transfer. Superhydrophobic surfaces provide an effective approach but suffer from phase change-induced wetting transitions, hindering their practical applications. In this work, Biphilic armored superhydrophobic surfaces (BASS) are designed by integrating hydrophilic interconnected surface frames with superhydrophobic nanostructures. The hydrophilic top of the frame provides spatial selectivity for condensate droplet nucleation, and superhydrophobic nanostructures enable staying dry. Further growth, coalescence, jumping, and roll-off of the condensate droplets on BASS, show remarkable resistance to phase change-induced wetting transition. It still maintains stable superhydrophobicity when exposed to 100 °C of steam for 240 h, at least two orders of magnitude improvement over traditional superhydrophobic surfaces. Such a designing BASS provides an effective approach to address the phase change-induced wetting transition, thereby extending the practical application in the fields of condensation heat transfer, anti-fouling, and fluid transportation of superhydrophobic surfaces.

研究领域: 材料科学 · 界面科学
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BIOMACROMOLECULES · 2020 · IF 6.092

Ratiometric Fluorescent Mapping of pH and Glutathione Dictates Intracellular Transport Pathways of Micellar Nanoparticles

Zexuan Ding,Guhuan Liu,Jinming Hu

Visualization of intracellular transport pathways is crucial to investigate the internalization mechanism and understand the intracellular behavior of nanomaterials. Herein, we rationalized the design of micellar nanoparticles (NPs) for ratiometric fluorescent mapping of intracellular pH and glutathione (GSH), two essential parameters for maintaining normal cellular functions. Specifically, pH-sensitive naphthalimide-based probe (NPI) and pH-inert rhodamine B (RhB) were covalently labeled to double hydrophilic block copolymers (DHBCs) using the thiolactone chemistry, enabling the covalent attachment of NPI and RhB to one molecule with a redox-responsive disulfide linkage. The dually labeled DHBCs exhibited blue/orange dual emissions in acidic pH, which was further converted into green/orange dual emissions in neutral pH because of the deprotonation of NPI moieties and the sole green emission in the presence of GSH at neutral pH because of the decreased Förster resonance energy transfer efficiency between an NPI donor and an RhB acceptor as a result of GSH-mediated cleavage of disulfide bonds. These remarkable ratiometric fluorescence changes allowed for not only the simultaneous mapping of the intracellular pH and GSH but also the intracellular transport pathways of internalized NPs.

研究领域: 生物医学工程 · 分子生物学 · 纳米医学
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Polymer Chemistry · 2022 ·Vol. 13 ·期 19 ·2791-2802 · IF 5.364

A well-defined thermo- and pH-responsive double hydrophilic graft copolymer bearing pyridine-containing backbone

Rang Chen,Xue Jiang,Guolin Lu,Wenbin Liu,Weize Jin,Guojian Tian,Xiaoyu Huang

Graft copolymers have extensive applications in material science because of the tunable nature of their backbones and side chains and the diverse morphologies of their aggregates. Recent studies have mainly focused on amphiphilic graft copolymers containing hydrophobic backbones and hydrophilic side chains. To the best of our knowledge, no studies have reported amphiphilic graft copolymers bearing pyridine-containing hydrophilic backbones. Based on the design of functional monomers, a new trifunctional acrylate monomer, PyMCIBMA, was prepared in two steps via a Morita–Baylis–Hillman reaction, followed by reaction with 2-chloroisobutyryl chloride. Reversible addition–fragmentation chain transfer (RAFT) polymerization of PyMCIBMA monomer was performed to generate a well-defined poly(PyMCIBMA) homopolymer possessing a Cl-containing ATRP initiating group in each repeat unit. Next, a series of well-defined double hydrophilic graft copolymers bearing densely distributed poly(N-isopropyl acrylamide) (PNIPAM) side chains along the backbone on every unit, PPyMA-g-PNIPAM, was synthesized via atom transfer radical polymerization (ATRP) initiated by poly(PyMCIBMA) homopolymer. The resulting graft copolymers exhibited intriguing dual temperature- and pH-sensitive behavior, signifying their potential applications in controlled delivery as polymer–drug nanocarrier.

研究领域: 材料科学 · 高分子化学
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ANALYTICA CHIMICA ACTA · 2020 · IF 5.977

Bisphosphorylated fructose-modified magnetic Zr-Organic framework: A dual-hydrophilic sorbent for selective adsorption of immunoglobulin G

Zhengjie Hu,Ximing Wang,Xuwei Chen

Highly selective adsorption of protein species interested from complicated biological samples is an extremely important prerequisite for in-depth proteomic analysis. Herein, a novel dual-hydrophilic material is fabricated by grafting Zr-based metal-organic framework (Zr-MOF) onto the surface of magnetic microspheres , and subsequent modifying with fructose-1,6-bisphosphate (FBP) molecules by taking advantage of multivalent binding between the phosphate backbone of FBP and Zr centers. Owing to the favorable dual-hydrophilicity derived from the abundant amino groups in Zr-MOF and the hydroxyl groups in FBP molecules, the obtained magnetic microspheres (mMOF-FBP) provide high adsorption efficiency, favorable selectivity and excellent capturing capacity (555.6 mg g −1 ) towards immunoglobulin G (IgG). The captured IgG could be collected from the mMOF-FBP by using 0.5% (m/v) NH 3 ·H 2 O as elution reagent with a recovery of 88.4%. The dual-hydrophilic microspheres demonstrate their practicability by selective isolation of IgG from human serum.

研究领域: 生物化学 · 材料科学 · 蛋白质组学
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Nanoscale · 2018 ·Vol. 10 ·期 26 ·12487-12496 · IF 7.233

Mussel-inspired construction of thermo-responsive double-hydrophilic diblock copolymers-decorated reduced graphene oxide as effective catalyst supports for highly dispersed superfine Pd nanoparticles

Haichao Duan,Yu Yang,Jianhua Lü,Changli Lü

Well-dispersed ultrafine palladium nanoparticles supported by reduced graphene oxide functionalized with catechol-terminated thermo-responsive block copolymer (PdNPs@BPrGO) were successfully constructed for highly efficient heterogeneous catalytic reduction. We first synthesized a novel temperature-responsive episulfide-containing double-hydrophilic diblock copolymer, poly(poly(ethylene glycol) methyl ether methacrylate-co-2,3-epithiopropyl methacrylate)-block-poly(N-isopropylacrylamide) (P(PEGMA-co-ETMA)-b-PNIPAM), through a reversible addition–fragmentation chain transfer (RAFT) polymerization utilizing a chain-transfer agent with a catechol unit as the end group. The obtained block copolymers can be facilely anchored to the surface of GO via mussel-inspired chemistry. The PdNPs were loaded on GO decorated with block copolymer brushes (BPrGO) as a support via the in situ reduction of palladium precursors with the episulfide ligands of the block copolymer as a stabilizer. The resulting PdNPs@BPrGO nanohybrid catalyst had good water dispersibility and stability. Furthermore, a low dosage of PdNPs@BPrGO catalyst exhibited excellent catalytic performance in the reduction of methylene blue and nitrophenols. The performance was attributed to the ability of PdNPs@BPrGO to facilitate the diffusion of reactants compared to PdNPs@GO without polymer modification. PdNPs@BPrGO also possessed an interesting temperature-responsive catalytic property due to the reversible “coil-to-globule” phase transition behaviour of PNIPAM blocks onto the surface of catalyst. The PdNPs@BPrGO catalyst was successfully recovered and reused five times without any detectible loss in catalytic activity, demonstrating its great potential in a wide range of industrial catalytic applications.

研究领域: 材料科学 · 催化化学
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Hydrophobic sponge with superhydrophilic sites for the controlled capture of surfactant-stabilized emulsified oil droplets

Liya Wang,Kaiming Peng,Di Zhao,Xinyuan Peng,Xiangfeng Huang,Jia Liu,Chen Cai,Jing Kang,Shiyang Li

Hydrophobic sponges have been identified as a promising material for the recovery of floating or dispersed oil, but they still face challenges in recovering oil from surfactant-stabilized emulsions. In this study, the melamine sponge (MS) was modified with Fe 3 O 4 magnetic particles (MPs), forming a hydrophobic sponge skeleton interspersed with superhydrophilic particles, denoted as MP@MS. The hydrophilic sites of the sponge can attract and capture the emulsified oil droplets with the hydrophilic ends of the surfactants stretching into the aqueous phase; then oil droplets spread along the hydrophobic skeleton; thereby recovering surfactant-stabilized emulsified oil droplets. To prepare the dual-wettability sponge, dopamine/polyethyleneimine (DA/PEI) was used to achieve hydrophilic modification of MPs, hydrophobic modification of MS, and bond them together synchronously by a facile one-pot synthesis. Compared with traditional hydrophobic sponges, the separation efficiency for surfactant-stabilized emulsions treated by MP@MS can increase from 5 % to approximately 90 %. MP@MS can effectively capture both anionic and nonionic-stabilized emulsified oil droplets, among which, the controlled continuous capture can be realized for oil droplets stabilized by nonionic surfactant. Furthermore, nonionic surfactant-coated oil droplets were verified through molecular dynamics (MD) simulations that they were more likely to detach from hydrophilic sites, and in this process remove surfactant molecules. This was conducive to exposing the hydrophilic sites promptly and thus demulsifying continuously. The new design principles and processing strategies will support the development and application of materials with dual-wettability structures in many fields, such as oil recovery, smart separation, and liquid manipulation.

研究领域: 材料科学 · 环境科学
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