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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

pH/Hypoxia dual-stimuli responsive COF nanocarriers with reversible charge conversions for the accurate tumor-targeting and enhanced anticancer drug delivery

Zhihao Wang,Qiuli Cheng,Xingda Jiang,Xinyang Chu,Bingcan Li,Leitao Zhang,Wenlan Wu,Junbo Li,Ravin Narain

Nanoparticles-based drug delivery systems show great promise for cancer therapy due to the advantages of crossing physiological barrier, high drug availability and good stability. However, deep tumor penetration, long blood circulation, and rapid drug release remain intractable problems for nanocarriers. In this work, we report a tumor microenvironment-sensitive nanodrug delivery system containing both acidic pH and hypoxia response sites to achieve enhanced drug permeability and on-demand release for precise cancer therapy. The covalent organic frameworks (COFs) with introduced azobenzene (azo) groups were used as employed as nanocarrier, and modified by pH-sensitive sulfamide-based zwitterionic polymers (PBA), followed by loading with the chemotherapeutic drug doxorubicin (DOX) to obtain COF-PBA@DOX. Copolymer PBA achieved charge conversions in tumor acidic environment, resulting in a positive charge on the nanocarrier surfaces, thus facilitating the augmented tumor accumulation. Meanwhile, azo which was formed the COF carrier, could be reduced to amines by the highly expressed azoreductase under tumor hypoxia conditions, resulting in nanoparticle dissociation and the drug-controlled release at the solid tumor sites. The fabricated dual-responsive nanomedicine, based on the surface charge-reversal of zwitterion in the acidic environment of tumor, can realize the accumulation and targeted drug release at the tumor site, which has great potential as a nanocarrier in tumor therapy.

研究领域: 纳米技术 · 癌症研究 · 药物递送系统 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

yMoO42- modified amorphous Co(PO3)2 cubes as an efficient bifunctional electrocatalyst for alkaline overall water splitting

Dengke Zhao,Shunlian Ning,Xiaolong Yu,Qikai Wu,Wei Zhou,Jiacheng Dan,Yuguang Zhu,Hao Zhu,Nan Wang,Ligui Li

The exploration of efficient bifunctional electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) under alkaline conditions is an important   way to promote the development of electrolytic water technology . Herein, the reduced graphene oxide-supported MoO 4 2- modified amorphous cobalt metaphosphate cubes (a-Co(PO 3 ) 2 /MoO 4 /rGO) as bifunctional OER/HER catalyst is prepared by anion exchange and phosphating, using the Prussian blue analogue (PBA) as a precursor. The resulting composite exhibits the low overpotentials (η) that of 290 and 50 mV for OER and HER in 1.0 M KOH solution at 10 mA cm −2 , respectively. The electrochemical test and density functional theory (DFT) results reveal that the MoO 4 2- -modified optimizes the adsorption/desorption energy of H* of Co(PO 3 ) 2 , thus enhance the HER activity. Benefiting from efficient HER and OER performances, an efficient and stable alkaline water electrolysis operation using a-Co(PO 3 ) 2 /MoO 4 /rGO used as bifunctional catalyst can be carried out, which can deliver a current density (j) of 20 mA cm −2 at 1.65 V cell voltage and work continuously for 24 h.

研究领域: 电化学 · 材料科学 · 催化 · 可再生能源
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RSC Advances · 2017 ·Vol. 7 ·期 73 ·45978-45986 · IF 3.108

Novel amphiphilic glucose-responsive modified starch micelles for insulin delivery

Na Wen,Chunmei Gao,Shaoyu Lü,Xiubin Xu,Xiao Bai,Can Wu,Piao Ning,Shaofei Zhang,Mingzhu Liu

The high pKa (8.26 to 8.6) of PBA has restricted its glucose-responsiveness in physiological conditions, and the high cytotoxicity of polymers is also a limiting problem in their potential application for insulin delivery. Novel amphiphilic glucose-sensitive dialdehyde starch polymers containing 3-aminophenylboronic acid (APBA) as a glucose-responsive group and mPEGylated dialdehyde starch (mPEG-DAS) with hydrophobic 7-hydroxycoumarin-4-acetic acid (Cou) were synthesized. This dialdehyde starch derivative can self-assemble into mPEG-DAS–APBA–Cou micelles with “shell–core” structures in phosphate-buffered saline solution (PBS). In addition, the drug-loaded micelles can release insulin rapidly in response to hyperglycemia in a physiological environment. The results demonstrated that the mPEG-DAS–APBA–Cou micelles showed notable glucose responsive behavior near the physiological range. The insulin release from the nanocarriers is sensitive to different concentrations of glucose, releasing insulin rapidly under the conditions of 3 mg mL−1 glucose while demonstrating comparatively inert release at 1 mg mL−1 glucose (pH 7.4). MTT assays and hemolysis studies both confirmed that the mPEG-DAS–APBA–Cou micelles have low cytotoxic activity to A549 cells and low blood toxicity. These results suggest that the glucose-sensitive dialdehyde starch micelles (mPEG-DAS–APBA–Cou) have potential applications as a glucose-responsive material for insulin delivery.

研究领域: 药学 · 纳米技术 · 生物材料 · 药物递送系统
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Hydrothermal pre-anchoring and in-situ preparation of Prussian blue analogue-polymeric carbon nitride nanorods hybrid for robust and efficient cesium adsorption

Shangqing Chen,Deyun Sun,Lei Zou,Yi Huang,Fanpeng Cheng,Lijuan Shi,Abdullah Tasleem,Atta Ullah,Syed Sheraz Daood,Qun Yi

Prussian blue analogues (PBAs) are recognized as effective and selective adsorbents for Cs + , however, they suffered from unsatisfactory post-separation performance and inevitable dissolution loss arising from the small size and inferior water instability. In this study, Zn-PBA nanoparticles were integrated onto polymeric carbon nitride (PCN) nanorods to form PBA-PCN hybrid via hydrothermal pre-anchoring and in-situ growth method. The robust and amino-rich PCN played dual roles in securely anchoring the Zn 2+ precursor and attracting Cs + to the surface. Benefiting from the effects of PCN and in-situ generated PBA, PBA-PCN exhibited boosting post-separation performance and water stability in acid and alkaline solutions, which was attractive in different application scenarios. Moreover, PBA-PCN has been demonstrated to be with high adsorption capacity of 376.41 mg/g and favorable selectivity even in the presence of excessive competitive ions. The experimental results and DFT calculations suggested the adsorption mechanism involving strong incorporation/ion exchange and weak electrostatic attraction. The remarkable adsorption performance along with the satisfactory post-separation performance and water stability made it a promising candidate in Cs + removal and separation.

CAS / MDL: 108-78-1
研究领域: 材料科学 · 环境工程 · 化学工程 · 纳米技术
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Time-space regulating prodrug hydrogels for prevention of peritendinous adhesion

Zhipeng Ni,Haiying Zhou,Haojie Yu,Li Wang,Chenguang Ouyang,Jian Yang,Yanzhao Dong,Ahmad Alhaskawi,Tian Tu,Hui Lu

The bidirectional regulations of antiadhesion and regeneration are crucial for Achilles tendon injuries. However, the precise prevention and treatments of peritendinous adhesions both in time and space are still great challenges. Here, a series of time–space regulating prodrug (tannic acid (TA), epigallocatechin (EGC) and epigallocatechin gallate (EGCG)) hydrogels are designed for the prevention of peritendinous adhesion in Achilles tendon contusion and rupture injuries. In the term of space, the self-healing and deformable hydrogels prepared by crosslinking phenylboric acid (PBA) functionalized polyphosphazene (PZBA) with guar gum (GG) through ROS-responsive phenylborate ester (PBAE) can specifically aggregate to the high ROS sites via the ROS-responsive degradation and recombination of PBAE. Thus, providing support and acting as barriers to inhibit fibroblast proliferation. In the term of time, the prodrug strategy using ROS-responsive PBAE as bridging linker can achieve long-term anti-inflammatory effect over 2 weeks. Furthermore, the degradation time of hydrogels matched the course of peritendinous adhesion, thus achieved bidirectional regulations (decrease the gene expression of TGF-β1, COL-1 and COL-3 to antiadhesion in the early stage but increase them to promote regeneration in the late stage). This study presents a promising approach employing smart prodrug hydrogels with time–space regulating properties for prevention of peritendinous adhesion.

研究领域: 生物医学工程 · 药剂学 · 材料科学 · 组织工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Precursor design in a self-templating strategy for carbon-encapsulated bimetallic CoFe catalysts: Boosting organic pollutant degradation via nonradical pathways

Weixuan Guo,Sixiang Zhuang,Ying Peng,Yi Shen,Yungui Li,Suorong Zhang,Qile Fang

Designing high-performance heterostructure catalysts for peroxymonosulfate (PMS) activation is a promising research area. PMS-driven organic pollutant degradation via radical pathways usually suffers from the interference of other coexisting matters. In this study, we took a source design approach and employed a self-templating strategy using Prussian blue analog (PBA) precursors to fabricate CoFe/C heterostructure catalysts dominated by a nonradical pathway. Slow-speed coordination renders the CoFe PBA precursor with a highly ordered crystal structure and fewer coordinated water, resulting in an ideal carbon-encapsulated CoFe bimetallic catalyst (CoFe-S-T) with more high-valence metals and a graphitized carbon layer in its heterostructure; the obtained catalyst is proven to have superior catalytic performance for tetracycline (TC) degradation through a nonradical pathway in PMS-driven oxidation . The high Co III /Co II ratio and surface oxygen content make CoFe-S-T an excellent catalyst by boosting the generation of 1 O 2 , which is the predominant active species. In addition, CoFe-S-T has a high proportion of graphitized carbon layers, which significantly improves the direct electron transfer pathway. Thus, utilizing precursor design in a self-templating strategy is an effective method to synthesize high-performance heterostructures for PMS-driven organic pollutant degradation.

CAS / MDL: 10026-24-1 75-65-0
研究领域: 环境科学 · 材料科学 · 化学工程 · 催化
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Advanced Healthcare Materials · 2022 ·Vol. 12 ·期 1 ·2201594 · IF 11.092

An ECM-Mimicking, Injectable, Viscoelastic Hydrogel for Treatment of Brain Lesions

Yan Hu,Yuanbo Jia,Siwei Wang,Yufei Ma,Guoyou Huang,Tan Ding,Dayun Feng,Guy M. Genin,Zhao Wei,Feng Xu

Brain lesions can arise from traumatic brain injury, infection, and craniotomy. Although injectable hydrogels show promise for promoting healing of lesions and health of surrounding tissue, enabling cellular ingrowth and restoring neural tissue continue to be challenging. It is hypothesized that these challenges arise in part from the mismatch of composition, stiffness, and viscoelasticity between the hydrogel and the brain parenchyma, and this hypothesis is tested by developing and evaluating a self-healing hydrogel that not only mimics the composition, but also the stiffness and viscoelasticity of native brain parenchyma. The hydrogel is crosslinked by dynamic boronate ester bonds between phenylboronic acid grafted hyaluronic acid (HA-PBA) and dopamine grafted gelatin (Gel-Dopa). This HA-PBA/Gel-Dopa hydrogel could be injected into a lesion cavity in a shear-thinning manner with rapid hemostasis, high tissue adhesion, and efficient self-healing. In an in vivo mouse model of brain lesions, the multi-functional injectable hydrogel is found to support neural cell infiltration, decrease astrogliosis and glial scars, and close the lesions. The results suggest a role for extracellular matrix-mimicking viscoelasticity in brain lesion healing, and motivate additional experimentation in larger animals as the technology progresses toward potential application in humans.

研究领域: 神经科学 · 材料科学 · 生物材料 · 组织工程
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

In situ construction of 3D Li channels high-temperature-resistant polymer electrolyte and Li3N-rich interface enabling stable solid-state Li metal battery

Minhui Liao,Yang Zhou,Xunchang Jiang,Renjie Wan

High safety, high ion conductivity, and stable interface contacts are of significant importance for the application of solid-state electrolytes (SSEs) in solid-state lithium metal batteries (SSLMBs). In this study, SSEs with high ion conductivity and safety were constructed by in-situ polymerization of poly butyl acrylate (PBA) based electrolytes in the three-dimensional (3D) pores of a polyvinylidene fluoride (PVDF) nanofiber membrane, and embedded with ion conductor succinonitrile (SN), fluorinated ethylene carbonate (FEC), and imidazolium-based ionic liquid (IL). The test results and microscopic structural analysis indicate that SN is uniformly dispersed in PVDF, effectively reducing the crystallinity of solid polymer electrolytes (SPEs) and constructing a 3D interconnected lithium-ion conduction network. Consequently, an ion conductivity of 4.89 mS cm −1 was achieved at 25°C. Meanwhile, density functional theory (DFT) calculations demonstrated that imidazolium-based ionic liquid can adjust the dissolution characteristics of Li + through weak interactions with the polymer framework and strong coordination with TFSI - . X-ray photoelectron spectroscopy (XPS) characterization revealed that the imidazolium-based ionic liquid can form a stable solid electrolyte interface enriched with Li 3 N on the lithium-metal surface. The resulting SPEs demonstrated excellent ion conductivity, a high Li + transfer number (t Li + = 0.739), and a nanofiber-reinforced interpenetrating framework with a tensile strength of 17.15 MPa. Furthermore, the LiFePO 4 (LFP)||Li battery equipped with PBA-PVDF-SN (modified with IL) exhibited excellent electrochemical performance at room temperature with a capacity retention of 87.4 % after 800 cycles at 0.5C.

研究领域: 材料科学 · 电化学 · 电池技术 · 聚合物化学
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Polymer Chemistry · 2014 ·Vol. 5 ·期 21 ·6244-6255 · IF 5.368

Versatile RAFT dispersion polymerization in cononsolvents for the synthesis of thermoresponsive nanogels with controlled composition, functionality and architecture

Yuanyuan Xu,Youcheng Li,Xueteng Cao,Qijing Chen,Zesheng An

Reversible addition–fragmentation chain transfer (RAFT) dispersion polymerization in cononsolvents of poly(N-isopropylacrylamide) (PNIPAM) was developed as a versatile strategy for the synthesis of thermoresponsive nanogels with controlled composition, functionality and architecture. Cononsolvents composed of mixtures of methanol, ethanol and isopropanol with water were first screened for their suitability as the media for dispersion polymerization of NIPAM, and water–ethanol (75 : 25, v : v) solution was selected due to good RAFT control, efficient formation of nanogels and low toxicity. RAFT dispersion polymerization of NIPAM in the cononsolvent using poly(N,N-dimethylacrylamide) (PDMA) as the macromolecular chain transfer agent (Macro-CTA) showed good control over the molecular weight, polydispersity and pseudo linear polymerization kinetics, as characterized by gel permeation chromatography (GPC) and 1H NMR. The effect of the molecular weight of Macro-CTA, the degree of polymerization of PNIPAM, the molar ratio of [crosslinker] : [Macro-CTA] and the solid content on the formation and size of nanogels was investigated. The thermal profiles of nanogels were characterized by dynamic light scattering (DLS) both in cononsolvents and water. This cononsolvency strategy for dispersion polymerization was shown to be compatible with the incorporation of hydrophilic comonomers of N-(2-hydroxyethyl)acrylamide (HEAM) and diacetone acrylamide (DAAM). The nanogel containing DAAM was demonstrated for postpolymerization modification using ketone–alkoxyamine chemistry. More importantly, dispersion polymerization in cononsolvents allowed various hydrophobic components, e.g. butyl acrylate (BA), fluorescein O-acrylate (FLA), and 1,6-hexanediol diacrylate (HDDA), to be reliably copolymerized with NIPAM, showing well controlled polymerization, composition, nanogel size and colloidal stability. Finally, an amphiphilic block copolymer PDMA-b-PBA was used as a Macro-CTA to produce the PDMA-b-PBA-b-PNIPAM triblock copolymer and triple-layered nanogel, taking advantage of the solubility of PDMA-b-PBA and the insolubility of PNIPAM in the water–ethanol solution at the polymerization temperature.

CAS / MDL: 2873-97-4 13048-33-4
研究领域: 高分子化学 · 材料科学 · 纳米技术
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