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POLYMER · 2022 · IF 4.432

Flexible and mechanically robust polyimide foam membranes with adjustable structure for separation and recovery of oil-water emulsions and heavy oils

Xinyu Yao,Xianbo Hou,Rubing Zhang

Oil-water separation materials have been widely studied, however, these materials are mainly used to separate light oil-water mixtures, and the application of heavy oil separation and recovery is rarely involved. It is urgent to develop novel multi-functional oil-water separation materials, especially for the separation membrane for heavy oil. Herein, mechanically robust fiber-reinforced fluorinated polyimide foam membranes (FPIFMs) with adjustable multistage pore structure and high oil-water selectivity were prepared by freeze-drying and surface modification. FPIFMs exhibit high tensile strength of 3.80 MPa with the synergistic effect of PI fibers and PAA . Besides, the macro void structure of the foam membrane can be precisely adjusted to achieve the separation of different types of oil-water mixtures, oil-water emulsions, especially the separation and recovery of heavy oil. The results show that the foam membranes can separate light oil (26935L·m −2 ·h −1 ), oil-water emulsion (364L·m −2 ·h −1 ) and heavy oil (30L·m −2 ·h −1 ) under gravity. This stable, highly flexible, highly efficient and reusable foam membrane is an attractive option for oil spill treatment and wastewater purification.

CAS / MDL: 78560-45-9 1338-43-8
研究领域: 材料科学 · 环境工程 · 化学工程
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Materials Chemistry Frontiers · 2022 ·Vol. 6 ·期 10 ·1269-1281 · IF 8.683

A nano-catalyst promoting endogenous NO production to enhance chemotherapy efficacy by vascular normalization

Xiaohui Wang,Xiaoyue Feng,Mengjie Sun,Mingzhu Wang,Wei Wang,Zhi Yuan

Poor perfusion and low accumulation of drugs caused by abnormal tumor blood vessels significantly reduce the chemotherapy efficacy. Nowadays, the synergistic therapy of vascular normalization and chemotherapy has become an ideal choice to increase the tumor inhibition rate. Delivering an appropriate amount of NO around tumor vessels proved to be an effective vascular normalization strategy. In order to meet the demand for continuous and stable production of NO at the tumor site, herein, we developed a strategy to normalize tumor blood vessels by catalyzing NO generation from endogenous NO donors (RSNO). Concretely, the surface of copper-doped mesoporous silica was modified with PAA by electrostatic interactions to form CuMSN-PAA nanoparticles. The system was simple in structure and could catalyze NO production by exposing the CuMSN surface in response to a slightly acidic environment. In vivo, the NO level in the tumor increased 5.8-fold after CuMSN-PAA treatment, and blood perfusion increased by 70%, which in turn induced vascular normalization. Consequently, DOX accumulation of the CuMSN-PAA group increased 2.4-fold compared with the control group. More importantly, after the synergistic treatment of vascular normalization and chemotherapy, the anti-tumor efficacy was increased by 37.2% compared with the DOX-treated group with no overt toxicity observed.

CAS / MDL: 25316-40-9 47165-04-8
研究领域: 癌症治疗 · 纳米技术 · 药学 · 生物医学工程
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International Journal of Nanomedicine · 2025 · IF 6.5

Acid-Unlocked Two-Layer Ca-Loaded Nanoplatform to Interfere With Mitochondria for Synergistic Tumor Therapy

Yilu Zheng,Gareth R Williams,Ran Hu,Sen Tong,Jianxiang Xu,Tong Wang,Yanyan Zhang,Junzi Wu,Fan Li,Yingyu Cai,Li-Min Zhu

Background: The development of selective formulations able to target and kill tumor cells without the application of external energy has shown great promise for anti-tumor therapy.Methods: Here, we report a “nanobomb” that explosively increases Ca content within cells. It can selectively release Ca2+ and generate H2O2 in the tumor microenvironment (TME) by acid-triggered degradation of the two-layer protective shell (ie, unlocking the “double-lock”). This material, termed CaO2@ZIF8:CUR@PAA, comprises a CaO2 core coated with the ZIF-8 framework, which was then loaded with curcumin (CUR) and coated again with polyacrylic acid (PAA).Results: Under the slightly acidic conditions of the TME, the PAA shell (first lock) breaks down first exposing CaO2@ZIF8 and CUR inside the cell. Then, ZIF8 (second lock) is degraded in response to acid to deposit Ca2+, and H2O2. CUR can promote the release of Ca2+ from the endoplasmic reticulum to the cytoplasm, inhibit the outflow of Ca2+, and accumulates a large amount of Ca2+ intracellularly together with exogenous Ca2+ (calcium storms). The powerful calcium storm that causes mitochondrial dysfunction. The presence of a large amount of exogenous H2O2 causes further oxidative damage to tumor cell membranes and mitochondria where intracellular ROS production far exceeds clearance. CaO2@ZIF8:CUR@PAA NPs can induce cell S cycle arrest and apoptosis to inhibit tumor multiplication and growth. Oxidative damage-triggered immunogenic cell death (ICD) in turn leads to the polarization of macrophages to the M1 phenotype, inducing immunogenic cell death and inhibiting tumor cell proliferation and metastasis.Discussion: The acid two-step unlocking nanoplatform is a therapeutic modality that combines calcium storm and oxidative damage. The mode triggers apoptosis leading to ICD of tumor cells. The material induces cycle blockade during treatment to inhibit cell proliferation. Robust in vitro and in vivo data demonstrate the efficacy of this approach and CaO2@ZIF8:CUR@PAA as an anticancer platform, paving the way for nanomaterials in immune-triggered cancer therapy.Highlights: - A new calcium accumulation nanoplatform plays a role in activate antitumor immunity.- Double-locked structure slows down the premature decomposition of CaO2.- The platform allows Ca2+ and H2O2 to accumulate in tumor cells.- This leads to mitochondrial dysfunction, apoptosis, and M1 macrophage polarization.- Potent anti-tumor effects are seen both in vitro and in vivo.

研究领域: 癌症治疗 · 纳米技术 · 免疫学 · 细胞生物学 · 药理学
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

Comparative study of block copolymer-templated localized surface plasmon resonance optical fiber biosensors: CTAB or citrate-stabilized gold nanorods

Mengdi Lu,Hu Zhu,Ming Lin,Fang Wang,Long Hong,Jean-Francois Masson,Wei Peng

Block copolymer (BCP) brush-like layer absorbed on optical fibers are shown to address the longstanding challenge of forming dense and well-dispersed gold nanorods (AuNRs) films on highly curved surface, allowing the development of real-time localized surface plasmon resonance (LSPR) biosensors for antigen-antibody interaction. This method requires only solution-based manufacturing processes and a plasma cleaning step to self-assemble AuNRs with various aspect ratios on the optical fibers. Because AuNRs capped with cetyltrimethylammonium bromide (CTAB) have been problematic for biosensing applications due to their cytotoxicity and displacement difficulty in the construction of biosensors, citrate-stabilized AuNRs were prepared from CTAB-stabilized AuNRs via surfactant exchange. For comparison, both a poly(styrene)- b -poly(acrylic acid) (PS- b -PAA) BCP template with CTAB-stabilized AuNRs and a poly(styrene)- b -poly(4-vinyl pyridine) (PS- b -P4VP) BCP template with citrate-stabilized AuNRs were employed for the fabrication of the optical fiber biosensor. The LSPR spectral analysis results demonstrate that the sensitivity of the sensor produced by the PS- b -P4VP templating method was 1.5 times better than that of the sensor produced by the PS- b -PAA templating method, which was due to the improved surface coverage and reduced aggregation of nanoparticles. The detection limit of the PS- b -P4VP-templated sensor for human IgG was 0.6 nM. Furthermore, for citrate-stabilized AuNRs, the PS- b -P4VP templating method also led to a better surface morphology and higher sensitivity as compared to the standard particle absorption methods using alkoxysilanes or polyelectrolytes on identical fibers. The simplicity of the fabrication process and the far superior optical performance of the PS- b -P4VP-templated LSPR optical fiber sensor illustrate the ability to regulate the detection range by tuning the aspect ratios of the AuNRs, and demonstrate its application prospects as a real-time biosensor without cytotoxicity.

研究领域: 材料科学 · 纳米技术 · 光学传感 · 生物传感器
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Tough Adhesion of Freezing- and Drying-Tolerant Transparent Nanocomposite Organohydrogels

Beibei Liu,Feibo Li,Pengying Niu,Huanjun Li

Tough hydrogels with strong wet adhesion have drawn extensive attention for various applications. However, it is still challenging to achieve both excellent wet adhesion and freezing- and drying-tolerance in hydrogels. In this study, we present tough transparent nanocomposite organohydrogels based on the glycerol–water binary solvent system in the presence of Al(OH)3 nanoparticles as a cross-linker. The resultant organohydrogels exhibited excellent tensile strength (∼0.9 MPa), high transparency (97%), superior anti-drying and anti-freezing properties, and good ionic conductivity. In particular, polyacrylic acid (PAA) was chosen as the bridging polymer to endow the organohydrogels with strong wet adhesion. The interfacial adhesion energy exceeded 2200 J m–2, which was ascribed to the synergy of ionic coordination and hydrogen bonds between the nanoparticles and carboxyl groups in PAA chains. Interestingly, based on the strong wet adhesion, the transparent organohydrogels can be assembled into hydraulically driven soft variable-focus lenses with long-term ambient stability. This work will provide a new insight into controlled wet adhesion ̵of hydrogel and have great potential for hydrogel-based functional devices with long-term ambient stability.

研究领域: 材料科学 · 化学工程 · 纳米技术 · 生物医学工程
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Adhesive, Antibacterial, Conductive, Anti-UV, Self-Healing, and Tough Collagen-Based Hydrogels from a Pyrogallol-Ag Self-Catalysis System

Min Zhang,Qili Yang,Tianshuo Hu,Lele Tang,Yonghao Ni,Lihui Chen,Hui Wu,Liulian Huang,Cuicui Ding

Recently, versatile hydrogels with multifunctionality have been widely developed with emerging applications as wearable and implantable devices. In this work, we reported novel versatile hydrogels by self-catalyzing the gelation of an interpenetrating polymer network consisting of acrylic acid (AA) monomers and GA-modified collagen (GCOL) in situ decorated silver nanoparticles (AgNPs). The resultant hydrogel, namely AgNP@GCOL/PAA, has many desirable features, including good mechanical properties (such as 123 kPa, 916%, and 1961 J m−2 for the fracture stress, strain and tearing energy) that match with those of animal skin, excellent self-healing performance, favorable conductivity and strain sensitivity as a flexible biosensor, and excellent antibacterial and anti-UV properties, as well as the strong adhesiveness on skin. Moreover, AgNP@GCOL/PAA showed excellent biocompatibility via in vitro cell culture. Remarkably, AgNP@GCOL/PAA displayed superior hemostatic properties with sharply decreasing blood loss for a mouse liver incision, closely related to its strong self-adhesion which produced anchoring strength to the bleeding site and thus formed a network barrier with liver tissue. This study provides new opportunities for the facile preparation of widely used multifunctional collagen-based hydrogels based on a simple pyrogallol-Ag system.

研究领域: 材料科学 · 生物医学工程 · 化学 · 纳米技术 · 伤口愈合 · 组织工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2022 · IF 8.025

Freeze-resistant, rapidly polymerizable, ionic conductive hydrogel induced by Deep Eutectic Solvent (DES) after lignocellulose pretreatment for flexible sensors

Yin Yan,Changliu He,Lihe Zhang,Huifeng Dong,Xu Zhang

In this paper, ternary DES (choline chloride, glycerol, Lewis acid) was used to pretreat lignocellulose, and the DES solution with dissolved lignin was utilized as the medium of hydrogel to prepare DES-based polyacrylic acid/polyvinyl alcohol (PAA/PVA) double network hydrogels with great mechanical properties, self-adhesion, and high electrochemical sensitivity. The entanglement of PAA with PVA chains, the covalent linkage between Al 3+ and PAA chains and the metal phenol network (MPN) formed by Al 3+ and lignin improved the mechanical properties of the hydrogels, enabling the prepared hydrogels to achieve a tensile strain of 400 % and an elongation at break of 150 kPa. Secondly, the introduction of DES solution endowed the hydrogel with excellent electrical sensing ability and anti-freezing property, so that the hydrogel still maintains good flexibility and ionic conductivity at −20 °C. It was also found that the above hydrogel can achieve a high gauge factor of 4.19 as a flexible sensor, which provides scientific ideas for the application of the pretreated DES solution in the field of flexible wearable.

研究领域: 材料科学 · 化学工程 · 生物医学工程 · 高分子科学
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2019 · IF 1.911

Gradient nanoporous phenolics as substrates for high-flux nanofiltration membranes by layer-by-layer assembly of polyelectrolytes

Yazhi Yang,Qianqian Lan,Yong Wang

Thin film composite (TFC) membranes represent a highly promising platform for efficient nanofiltration (NF) processes. However, the improvement in permeance is impeded by the substrates with low permeances. Herein, highly permeable gradient phenolic membranes with tight selectivity are used as substrates to prepare TFC membranes with high permeances by the layer-by-layer assembly method. The negatively charged phenolic substrates are alternately assembled with polycation polyethylenimine (PEI) and polyanion poly(acrylic acid) (PAA) as a result of electrostatic interactions, forming thin and compact PEI/PAA layers tightly attached to the substrate surface. Benefiting from the high permeances and tight surface pores of the gradient nanoporous structures of the substrates, the produced PEI/PAA membranes exhibit a permeance up to 506 L   ∙   m −2   ∙   h −1   ∙   MPa −1 , which is ~   2–10 times higher than that of other membranes with similar rejections. The PEI/PAA membranes are capable of retaining >   96.1% of negatively charged dyes following the mechanism of electrostatic repulsion. We demonstrate that the membranes can also separate positively and neutrally charged dyes from water via other mechanisms. This work opens a new avenue for the design and preparation of high-flux NF membranes, which is also applicable to enhance the permeance of other TFC membranes.

CAS / MDL: 64-17-5 9002-98-6
研究领域: 材料科学 · 纳米技术 · 膜技术 · 环境工程
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Biotechnology Journal · 2022 ·Vol. 17 ·期 9 ·2200098 · IF 5.726

Microfluidic fabrication of tunable alginate-based microfibers for the stable immobilization of enzymes

Wen Zhang,Wenbo Ye,Yajun Wang,Yunfeng Yan

Immobilized enzymes have drawn extensive attention due to their enhanced stability, easy separation from reaction mixture, and prominent recyclability. Nevertheless, it is still an ongoing challenge to develop potent immobilization techniques which are capable of stable enzyme encapsulation, minimal loss of activity, and modulability for various enzymes and applications. These microfibers were able to efficiently encapsulate bovine serum albumin (BSA), glucose oxidase (GOx), and horseradish peroxidase (HRP). But the physically adsorbed enzymes readily diffused into the catalytic reaction system. The leakage of enzymes could be substantially inhibited by conjugating to poly(acrylic acid) (PAA) and incorporating into alginate-based microfibers, enabling stable immobilization, improved recyclability, and enhanced thermostability. In addition, GOx and HRP-loaded microfibers were fabricated under the optimized conditions for the visual detection of glucose using the cascade reaction of these enzymes, showing sensitive color change to glucose with concentration range of 0–2 m m . Due to the tunability and versatility, this microfluidic-based microfiber platform may provide a valuable approach to the enzyme immobilization for the cascade catalysis and diagnoses with multiple clinical markers. Graphical and Lay Summary Development of potent techniques for the immobilization of enzymes with stable encapsulation, minimal loss of activity, and good reusability is an ongoing challenge. In this study, authors developed co-flow microfluidic devices for the fabrication of alginate-based microfibers with tunable size and crosslinking degree for the stable immobilization of glucose oxidase and horseradish peroxidase. This microfluidic platform has great potential in the construction of customizable enzyme-loaded microfibers for the cascade catalysis and diagnoses with multiple clinical markers.

CAS / MDL: 25952-53-8 6066-82-6
研究领域: 生物化学 · 生物技术 · 材料科学 · 分析化学
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FUEL · 2024 · IF 6.7

Methane hydrate formation promoted by eco-friendly hydrogels carrying with trace SDS

Chang Li,Kang Tan,Fangzheng Hua,Changxue Wang,Xiaolin Wang,Fei Wang,Mengting Sun

Hydrate-based natural gas storage and transportation is in urgent need of efficient and eco-friendly promotion methods. Here, we employed a kind of eco-friendly hydrogels, which were polyvinyl alcohol-co-acrylic acid (PVA-co-PAA), as carriers for trace SDS solution to construct a co-promoter for methane hydrate formation. Under static condition without stirring, trace SDS solution that was lower than or equal to 0.4 mmol L −1 had no or had extremely weak promoting effects on hydrate formation kinetics, whereas hydrogel-carried trace SDS exhibited excellent synergistic promoting effects. The HS-0.4 under a SDS concentration of 0.4 mmol L −1 and at a swelling ratio of 200 g g −1 achieved the most remarkable promotion, and the induction time was 0 min, the hydrate growth rate at t 90 was 0.1552 ± 0.0068 mmol mL −1 min −1 , the methane uptake was 121.70 ± 1.58 mmol mol −1 and the water-to-hydrate conversion was 0.730 ± 0.009. During synergistic promotion process, on the one hand, hydrogels keeping with large surface area increased gas–liquid interface, and were in charge of facilitating hydrate nucleation and shortening induction time; on the other hand, trace SDS produced strong capillary effect and sharply boosted mass transfer during hydrate growth period, which drastically enhanced hydrate growth rate and methane uptake. Morphology observation on hydrate evolutions unveiled that the co-promoter significantly improved poor hydrate compactness and partly relieved foam problem caused by SDS. Hydrogel-carried trace SDS can serve as an effective, eco-friendly and economical promotion approach for methane hydrate formation, which might be of great benefit for hydrate-based natural gas storage and transportation.

CAS / MDL: 9002-89-5
研究领域: 化学工程 · 材料科学 · 环境科学 · 能源存储与运输
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-19 · IF 16.6

Hypersensitive MR angiography based on interlocking stratagem for diagnosis of cardiac-cerebral vascular diseases

Zhang Peisen,Cheng Junwei,Lu Yijie,Zhang Ni,Wu Xiaoai,Lin Hua,Li Wei,Wang Jian,Winnik Mitchell A.,Gan Zhihua,Hou Yi

Magnetic resonance (MR) angiography is one of the main diagnostic approaches for cardiac-cerebral vascular diseases. Nevertheless, the non-contrast-enhanced MR angiography suffers from its intrinsic problems derived from the blood flow-dependency, while the clinical Gd-chelating contrast agents are limited by their rapid vascular extravasation. Herein, we report a hypersensitive MR angiography strategy based on interlocking stratagem of zwitterionic Gd-chelate contrast agents (PAA-Gd). The longitudinal molar relaxivity of PAA-Gd was 4.6-times higher than that of individual Gd-chelates as well as appropriate blood half-life (73.8 min) and low immunogenicity, enabling sophisticated micro-vessels angiography with a resolution at the order of hundred micrometers. A series of animal models of cardiac-cerebrovascular diseases have been built for imaging studies on a 7.0 T MRI scanner, while the clinical translation potential of PAA-Gd has been evaluated on swine on a 3.0 T clinical MRI scanner. The current studies offer a promising strategy for precise diagnosis of vascular diseases.

研究领域: 医学影像 · 血管疾病 · 磁共振血管成像 · 造影剂
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ACS Omega · 2020 · IF 2.87

Novel Modification of Collagen: Realizing Desired Water Solubility and Thermostability in a Conflict-Free Way

Junhui Yang,Cuicui Ding,Lele Tang,Feng Deng,Qili Yang,Hui Wu,Lihui Chen,Yonghao Ni,Liulian Huang,Min Zhang

Because of poor water solubility and low thermostability, the application of collagen is limited seriously in fields such as injectable biomaterials and cosmetics. In order to overcome the two drawbacks simultaneously, a novel bifunctional modifier based on the esterification of polyacrylic acid (PAA) with N-hydroxysuccinimide (NHS) was prepared. The esterification degree of PAA-NHS esters was increased upon increasing the NHS dose, which was confirmed by Fourier-transform infrared (FTIR) and nuclear magnetic resonance spectrascopy. FTIR results indicated that the triple helix of the modified collagens remained integrated, whereas the molecular weight became larger, as reflected by the sodium dodecyl sulfate–polyacrylamide gel electrophoresis pattern. The modified collagens displayed excellent water solubility under neutral condition, owing to lower isoelectric point (3.1–4.3) than that of native collagen (7.1). Meanwhile, denaturation temperatures of the modified collagens were increased by 4.8–5.9 °C after modification. The modified collagen displayed hierarchical microstructures, as reflected by field-emission scanning electron microscopy, while atomic force microscopy further revealed a “fishing net-like” network in the nanoscale, reflecting a unique aggregation behavior of collagen macromolecules after modification. As a whole, the PAA-NHS ester as a bifunctional modifier endowed collagen with desired water solubility and thermostability in a conflict-free manner, which was beneficial to the process and application of the water-soluble collagen.

研究领域: 生物材料 · 化妆品 · 材料科学 · 化学工程
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