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Self-assembling, pH-responsive nanoflowers for inhibiting PAD4 and neutrophil extracellular trap formation and improving the tumor immune microenvironment

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Acta Pharmaceutica Sinica B 2022年第5期12卷 2592-2608页

作者： Di Zhu Yu Lu Lin Gui Wenjing Wang Xi Hu Su Chen Yanming Wang Yuji Wang Department of Medicinal Chemistry College of Pharmaceutical Sciences of Capital Medical UniversityBeijing 100069China Beijing Area Major Laboratory of Peptide and Small Molecular Drugs Engineering Research Center of Endogenous Prophylactic of Ministry of Education of ChinaBeijing Laboratory of Biomedical MaterialsBeijing 100069China Beijing Institute of Hepatology Beijing Youan HospitalCapital Medical UniversityBeijing 100069China Quantum Design China Ltd. Universal Business ParkBeijing 100015China Laboratory of Biomaterials and Biomechanics Beijing Key Laboratory of Tooth Regeneration and Function ReconstructionSchool of StomatologyCapital Medical UniversityBeijing 100050China School of Life Sciences Henan UniversityKaifeng 475004China

Self-assembling carrier-free nanodrugs are attractive agents because they accumulate at tumor by an enhanced permeability and retention(EPR) effect without introduction of inactive substances,and some nanodrugs can alter the immune environment. We synthesized a peptidyl arginine deiminase 4(PAD4) molecular inhibitor, ZD-E-1 M. It could self-assembled into nanodrug ZD-E-1. Using confocal laser scanning microscopy, we observed its cellular colocalization, PAD4 activity and neutrophil extracellular traps(NETs) formation. The populations of immune cells and expression of immune-related proteins were determined by single-cell mass cytometry. ZD-E-1 formed nanoflowers in an acidic environment, whereas it formed nanospheres at pH 7.4. Accumulation of ZD-E-1 at tumor was pHresponsive because of its pH-dependent differences in the size and shape. It could enter the nucleus and bind to PAD4 to prolong the intracellular retention time. In mice, ZD-E-1 inhibited tumor growth and metastasis by inhibiting PAD4 activity and NETs formation. Besides, ZD-E-1 could regulate the ratio of immune cells in LLC tumor-bearing mice. Immunosuppressive proteins like LAG3 were suppressed,while IFN-γ and TNF-a as stimulators of tumor immune response were upregulated. Overall, ZD-E-1 is a self-assembling carrier-free nanodrug that responds to pH, inhibits PAD4 activity, blocks neutrophil extracellular traps formation, and improves the tumor immune microenvironment.

关键词： pH-Response Self-assembly Carrier-free nanoflowers Neutrophil extracellular traps Single-cell mass cytometry Tumor immune microenvironment Lymphocyte activation gene-3

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Facile self-template fabrication of hierarchical nickel-cobalt phosphide hollow nanoflowers with enhanced hydrogen generation performance

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Science Bulletin 2019年第22期64卷 1675-1684页

作者： Xupo Liu Shaofeng Deng Peifang Liu Jianing Liang Mingxing Gong Chenglong Lai Yun Lu Tonghui Zhao Deli Wang Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China Analysis&Testing Center of Xin yang Normal University Xin yang 464000.China

Developing facile methods to construct hierarchical-structured transition metal phosphides is beneficial for achieving high-efficiency hydrogen evolution catalysts.Herein,a self-template strategy of hydrothermal treatment of solid Ni-Co glycerate nanospheres followed by phosphorization is delivered to synthesize hierarchical Ni Co P hollow nanoflowers with ultrathin nanosheet assembly.The microstructure of Ni Co P can be availably tailored by adjusting the hydrothermal treatment temperature through affecting the hydrolysis process of Ni-Co glycerate nanospheres and the occurred Kirkendall effect.Benefitting from the promoted exposure of active sites and affluent mass diffusion routes,the HER performance of the Ni Co P hollow nanoflowers has been obviously enhanced in contrast with the solid Ni Co P nanospheres.The fabricated Ni Co P hollow nanoflowers yield the current density of 10 m A cmà2at small overpotentials of 95 and 127 m V in 0.5 mol Là1H2SO4and 1.0 mol Là1KOH solution,respectively.Moreover,the two-electrode alkaline cell assembled with the Ni Co P and Ir/C catalysts exhibits sustainable stability for overall water splitting.The work provides a simple but efficient method to regulate the microstructure of transition metal phosphides,which is helpful for achieving high-performance hydrogen evolution catalysts based on solid-state metal alkoxides.

关键词： Self-template method Hydrolysis of glycerate nanospheres Kirkendall effect NiCoP hollow nanoflowers Hydrogen evolution reaction

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Palladium nanoflowers supported on amino-fullerene as novel catalyst for reduction of 4-nitrophenol

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Chinese Chemical Letters 2020年第3期31卷 818-820页

作者： Zhongping Li Chunxiao Han Institute of Environmental Science Shanxi UniversityTaiyuan 030006China

In this study,we report the synthesis of novel palladium nanoflowers(Pd NFs)on amino-functionalized fullerene(C60-NH2)by hydrothermal self-assembly growth using ethylenediamine(EA)as a functional reagent.The successful formation of Pd nanoflowers supported amino-functionalized fullerene(C60-NH2/Pd NFs)is evidenced by UV-vis and powder X-ray diffraction(XRD).The morphology of Pd NFs over the C60-NH2 surface has been investigated by high-resolution transmission electron microscopy(TEM)and Fourier-transform infrared(FT-IR)techniques.The supported Pd nanoflowers(Pd NFs/C60-NH2)exhibit remarkably superior catalytic activity toward the reduction of 4-nitrophenol(4-NP).It exhibits remarkable UV-vis spectra response from 4-nitrophenol to 4-aminophenol(4-AP)(99%in 2.0 min)with a turnover frequency of 12.35 min^-1.Its excellent catalytic stability and durability offer the promising application in catalysis.

关键词： Palladium nanoflowers Self-assembly 4-Nitrophenol Amino-functionalized fullerene Catalyst

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Highly selective electrochemical method for the detection of serotonin at carbon fiber microelectrode modified with gold nanoflowers and overoxidized polypyrrole

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Chinese Chemical Letters 2019年第9期30卷 1643-1646页

作者： Jiajia Song Lifen Wang Hetong Qi Honglan Qi Chengxiao Zhang Key Laboratory of Analytical Chemistry for Life Science of Shaanxi Province School of Chemistry and Chemical Engineering Shaanxi Normal University Xi'an 710062 China Department of Applied Chemistry School of Science Xi'an Jiaotong University Xi'an 710049 China

A highly selective and sensitive electrochemical method was developed for the detection of serotonin (5-hydroxytryptamine, 5-HT) at gold nanoflowers (Au NFs) and overoxidized polypyrrole (OPPy) modified carbon fiber microelectrode (CFME). Carbon fiber was firstly modified with gold nanoflowers using electroless deposition method, and then modified with overoxidized polypyrrole using electrochemical polymerization and overoxidization to obtain OPPy/Au NFs/CFME. The obtained OPPy/Au NFs/CFME was characterized by field emission scanning electron microscopy and electrochemical techniques. It was found that the OPPy/Au NFs/CFME showed good sensitivity for the detection of 5-HT in the range of 10 nmol/L-7.0μmol/L with detection limit of 2.3 nmol/L, and negligible interferences from ascorbic acid, 5-hydroxyindole acetic acid and uric acid. The OPPy/Au NFs/CFME was successfully applied to the detection of 5-HT in human serum samples with good recovery. The work demonstrates that the electrochemical method, incorporating signal amplification of Au NFs with higher cation selection of OPPy, provides a promising tool for the detection of 5-HT in biological systems.

关键词： Serotonin Gold nanoflowers Overoxidized polypyrrole Carbon fiber microelectrode Electroless deposition

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A dual enzyme-phosphate hybrid nanoflower for glutamate detection

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Particuology 2023年第12期83卷 63-70页

作者： Peikun Li Jiahui Jia Zixin Geng Saizhao Pang Ruirui Wang Muhammad Bilal Hongjie Bian Jiandong Cui Shiru Jia State Key Laboratory of Food Nutrition and Safety Laboratory of Industrial Fermentation MicrobiologyMinistry of EducationTianjin University of Science and TechnologyTianjin300457China Research Center for Fermentation Engineering of Hebei College of Bioscience and BioengineeringHebei University of Science and TechnologyShijiazhang050000China Institute of Chemical Technology and Engineering Faculty of Chemical TechnologyPoznan University of TechnologyBerdychowo 4PL-60695PoznanPoland

The enzyme hybrid nanoflower has gained interests in biosensors due to their simple synthesis and high efficiency.In this study,glutamate oxidase(GLOX)and horseradish peroxidase(HRP)hybrid nanoflowers(GLOX&HRP-HNFs)were successfully prepared for the detection of glutamic acid(Glu).The effects of the synthesis conditions on the activity of GLOX&HRP-HNFs were investigated.Results revealed that the maximum activity of GLOX&HRP-HNFs was under 4 mM phosphate radical,2.5 mM MnSO4,0.04 mg/mL GLOX,and 0.16 mg/mL HRP.After immobilization,no significant differences were observed in optimum pH and temperature values of the GLOX and HRP.The GLOX&HRP-HNFs exhibited higher storage stability and resistance to organic solvents than free GLOX and HRP.Additionally,the GLOX&HRP-HNFs maintained 69%of its primary activity after 6 cycles.More important,the GLOX&HRP-HNFs exhibited a good linear range from 1 to 100μM(R^(2)=0.9979)and a low limit of detection(LOD)of 0.59μM for glutamate.These results suggest that the GLOX&HRP-HNFs is a promising candidate for applications in biosensing for the detection of glutamate.

关键词： Glutamate oxidase Horseradish peroxidase nanoflowers Glutamate detection

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In-Situ Chemosynthesis of ZnO Nanoparticles to Endow Wood with Antibacterial and UV-Resistance Properties

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Journal of Materials Science & Technology 2017年第3期33卷 266-270页

作者： Youming Dong Yutao Yan Huandi Ma Shifeng Zhang Jianzhang Li Changlei Xia Sheldon Q.Shi Liping Cai MOE Key Laboratory of Wooden Material Science and Application Beijing Forestry University Beijing 100083 China College of Biological Science and Technology Beijing Forestry University Beijing 100083 China Department of Mechanical and Energy Engineering University of North Texas 3940 N Elm St. Suite F101 Denton TX 76207 United States

Hybrid wood materials have attracted considerable attention because they have combined advantages of both wood and inorganic compounds. This work investigated the microstructural morphology, thermal stability, ultraviolet（UV） stability, and antibacterial property of composites made from wood/ZnO hybrid materials through a facile in-situ chemosynthesis methods. The X-ray diffraction（XRD） and thermogravimetric analysis（TGA） results indicated that the synthesized ZnO particles had an average grain size of about 10.8 nm. The scanning electron microscopy（SEM） observations showed that ZnO nanoflowers self-assembled with nanosheets were presented in wood cell lumens and increased with increasing Zn^（2＋）concentrations. ZnO nanoparticles were also generated in the wood cell wall, which was confirmed by the results of energy-dispersive spectroscopy（EDS）. The TGA tests also indicated that the thermal stability of wood/ZnO hybrid materials was improved after the formation of ZnO inorganic particles. Finally, the results of antibacterial efficacy tests and UV resistance tests revealed that ZnO nanoparticles showed a promising future as antimicrobial agents against Escherichia coli（E.coli） and UV resistance agents for wood protection.

关键词： Hybrid wood material nanoflowers Zinc oxide Antibacterial property UV-resistance

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Controlled Growth of Well-Aligned Carbon Nanotubes, Electrochemical Modification and Electrodeposition of Multiple Shapes of Gold Nanostructures

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Materials Sciences and Applications 2013年第11期4卷 667-678页

作者： Haniyeh Fayazfar Abdollah Afshar Abolghasem Dolati Department of Materials Science and Engineering Sharif University of Technology Tehran Iran

An efficient method has been developed to synthesize well-aligned multi-walled carbon nanotubes (MWCNTs) on a conductive Ta substrate by chemical vapour deposition (CVD). Free-standing MWCNTs arrays were functionalized through electrochemical oxidation with the formation of hydroxyl and carboxyl functional groups. Using a new oven drying technique, we demonstrate that the unidirectionally aligned and laterally spaced geometry of the CNT arrays can be retained after being subjected to each step of electrochemical modification. Samples were analyzed by using a field emission scanning electron microscope (SEM), transmission electron microscope (TEM), Fourier transformed infrared (FTIR) and Raman spectroscopy. Useful electrochemical methods for the synthesis of various gold nanostructures onto the aligned MWCNTs were then presented for the first time. The results demonstrated that flowerlike nanoparticle arrays, nanosheets and nanoflowers were obtained on the aligned CNTs under different experimental conditions. These kinds of aligned-CNT/Au nanostructures hybrid materials introduced by these efficient and simple electrochemical methods could lead to development of a new generation device for ultrasensitive catalytic and biological application.

关键词： Chemical Vapour Deposition Vertically Aligned Carbon Nanotube Electrochemical Techniques Nanostructures nanoflowers

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