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脂质化mno2仿生纳米黏膜佐剂的构建及其增强H1N1疫苗免疫效力评价

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脂质化MnO2仿生纳米黏膜佐剂的构建及其增强H1N1疫苗免疫效力评价

作者：程航航河南农业大学

学位级别：硕士

甲型H1N1也称猪流感（Swine influenza,SI）,是由A型流感病毒所引起的一种急性呼吸道传染病,是一种人畜共患病,具有高度传染性和变异性,对公共卫生和经济发展都造成了巨大的负担。鼻腔是流感病毒感染机体的主要部位,如果在鼻腔建立良好... 详细信息

甲型H1N1也称猪流感（Swine influenza,SI）,是由A型流感病毒所引起的一种急性呼吸道传染病,是一种人畜共患病,具有高度传染性和变异性,对公共卫生和经济发展都造成了巨大的负担。鼻腔是流感病毒感染机体的主要部位,如果在鼻腔建立良好的黏膜免疫,则可迅速有效地阻断病毒的感染。鼻内接种灭活疫苗是预防流感病毒感染的有效措施之一,但由于鼻腔纤毛的快速清除及黏膜下树突状细胞（Dendritic cells,DCs）数量不足,单独的灭活疫苗免疫效果并不理想。基于以上问题,设计了一种脂质化mno2仿生纳米黏膜佐剂(NLipo Mn)用于H1N1灭活疫苗（IIV）的鼻内免疫。与单独使用IIV相比,NLipo Mn明显延长了IIV的鼻腔滞留时间,提高黏膜上皮细胞分泌趋化因子CCL20的能力,从而促进黏膜下DCs的募集,促进了DCs对IIV的摄取。此外,NLipo Mn-IIV中的MNK、mno2可协同促进DCs成熟,T细胞活化和B细胞成熟,分泌高水平HA特异性Ig G及Ig A,从而产生强大的黏膜、细胞及体液免疫应答,实现对同源和异源H1N1流感病毒感染的有效保护。具体研究内容如下所示:1.纳米佐剂的制备和表征。首先,通过薄膜水合法及超声挤压法合成了NLipo Mn。动态光散射（DLS）结果显示NLipo Mn的粒径为246 nm,Zeta电位为+21 m V。紫外-可见光谱、FT-IR光谱、透射电子显微镜（TEM）图像及能量色散光谱（EDS）图像结果表明mno2被成功包裹。激光共聚焦显微镜（CLSM）图像、SDS-PAGE及WB结果表明MNK被成功融合。在吸附IIV后,NLipo Mn-IIV的粒径为350 nm,Zeta电位为+14 m V,HA含量为84.9μg/mg NLipo Mn-IIV。此外,在PBS或含10%FBS的1640培养基中孵育7天后粒径无明显变化,表明NLipo Mn及NLipo Mn-IIV具有良好的稳定性。2.体外DCs成熟。使用荧光标记的纳米疫苗与DCs共孵育,CLSM图像、流式细胞术与荧光定量结果表明NLipo Mn显著提高了DCs对IIV的摄取。此外,NLipo Mn-IIV可显著促进BMDCs表面CD80、CD86的表达和相关细胞因子（TNF-α,IL-12,IFN-γ,TNF-α）的分泌。这表明纳米疫苗具有强烈刺激DCs成熟的能力。3.黏膜下DCs的摄取。使用荧光标记的纳米疫苗分别鼻内接种小鼠观察其鼻腔滞留效果。小动物活体成像和CLSM图像显示NLipo Mn可促进IIV在鼻腔黏膜滞留。q PCR和流式细胞术结果表明NLipo Mn可促进趋化因子CCL20的分泌来招募DCs,进而增强DCs对IIV的摄取。4.纳米疫苗体内免疫效果。对小鼠进行滴鼻免疫后,NLipo Mn-IIV可有效刺激鼻腔组织及脾脏中DCs的成熟,T细胞的活化,B细胞的成熟,诱导产生高滴度的HA特异性Ig G及Ig A,并且表现出良好的生物安全性。5.纳米疫苗体内免疫保护效果。按照先前的免疫程序进行滴鼻免疫后,于初次免疫后第28天对小鼠进行流感病毒A/Puerto Rico/8/34（PR8,H1N1）或A/swine/Zhucheng/90/2014（ZC14,H1N1）攻毒。监测小鼠体重和存活率,并对攻毒后第5天的小鼠肺脏进行肺病理切片观察、肺指数评价及肺部病毒载量测定。结果表明,滴鼻免疫NLipo Mn-IIV的小鼠能够有效抵抗同源或异源流感病毒感染,表现为最高的存活率（100%）。综上所述,本文成功合成了一种脂质化mno2仿生纳米黏膜佐剂(NLipo Mn),NLipo Mn-IIV具有良好的体内外安全性,并可促进机体产生强烈的黏膜、体液及细胞免疫应答。在针对同源和异源H1N1流感病毒攻击时,显示出较其他制剂更强的保护效果。本研究为开发流感和其他呼吸道病毒感染的鼻内疫苗提供了一种有前景的、通用的纳米佐剂。

关键词：猪流感纳米黏膜佐剂 NK细胞膜 mno2 DCs募集协同免疫激活

Preparation of mno2 decorated Co3Fe1Ox powder/monolithic catalyst with improved catalytic activity for toluene oxidation

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Journal of Environmental Sciences 2020年第10期32卷 194-203页

作者： Tianshan xue Renna Li Zhang Zhang Yanshan Gao Qiang Wang College of Environmental Science and Engineering Beijing Forestry UniuersityBeijing 100083China Beijing Municipal Environmental Monitoring Center Beijing 100048China

In this paper, Kmno4 was used to pre-treat Co3 Fe-layered double hydroxides(LDH) precursor to prepare mno2 decorated Co3Fe1Ox catalyst. The toluene oxidation performance of the catalyst was investigated systematically. The optimized 0.1 Mn CF-LDO catalyst exhibited the best catalytic performance, and the temperatures of 50% and 90% toluene conversion( T50 and T90) were 218 and 243 ℃, respectively. The apparent activation energy( Ea) was 31.6 k J/mol. The characterization results showed that the pre-redox reaction by Kmno4 could increase the specific surface area, Co^3+ species amount and oxygen defect concentration of the catalyst, which are the main reason of the improved toluene catalytic activity. Besides, this method was also applied to enhance toluene oxidation of iron mesh based monolithic catalyst. The 0.1 Mn CF-LDO/Iron mesh(IM) catalyst showed a 90% toluene conversion at around 316 ℃ which was much lower than that of without mno2 addition(359 ℃). In addition, the water resistant of all the catalysts was studied as well, all the samples showed relatively good water resistance. The toluene conversion still remained to be over > 80% even in the presence of 10 vol.% water vapor.

关键词： Co3Fe-LDH mno2 Defective oxygen Toluene oxidation Monolithic catalyst

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Novel Insights into Energy Storage Mechanism of Aqueous Rechargeable Zn/mno2 Batteries with Participation of Mn2+

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Nano-Micro Letters 2019年第3期11卷 227-239页

作者： Yongfeng Huang Jian Mou Wenbao Liu Xianli Wang Liubing Dong Feiyu Kang Chengjun Xu Shenzhen Geim Graphene Center Graduate School at ShenzhenTsinghua UniversityShenzhen518055People’s Republic of China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing100084People’s Republic of China

Aqueous rechargeable Zn/mno2 zinc-ion batteries(ZIBs)are reviving recently due to their low cost,non-toxicity,and natural ***,their energy storage mechanism remains controversial due to their complicated electrochemical ***,to achieve satisfactory cyclic stability and rate performance of the Zn/mno2 ZIBs,Mn2+ is introduced in the electrolyte(e.g.,ZnSO4 solution),which leads to more complicated reactions inside the ZIBs ***,based on comprehensive analysis methods including electrochemical analysis and Pourbaix diagram,we provide novel insights into the energy storage mechanism of Zn/mno2 batteries in the presence of Mn2+.A complex series of electrochemical reactions with the coparticipation of Zn2+,H+,Mn2+,SO42-,and OH-were *** the first discharge process,co-insertion of Zn2+ and H+ promotes the transformation of mno2 into Znxmno4,mnoOH,and Mn2O3,accompanying with increased electrolyte pH and the formation of ZnSO4·3 Zn(OH)2-5 *** the subsequent charge process,Znxmno4,mnoOH,and Mn2O3 revert to a-mno2 with the extraction of Zn2+ and H+,while ZnSO4·3Zn(OH)2·5H2O reacts with Mn2+ to form ZnMn3O7·3 *** the following charge/discharge processes,besides aforementioned electrochemical reactions,Zn2+ reversibly insert into/extract from α-mno2,Znxmno4,and ZnMn3O7·3H2O hosts;ZnSO4·3Zn(OH)2·5 H2O,Zn2Mn3O8,and ZnMn2O4 convert mutually with the participation of Mn2+.This work is believed to provide theoretical guidance for further research on high-performance ZIBs.

关键词： Zinc-ion battery mno2 cathode Energy storage mechanism Phase evolution

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Synthesis of poly(3,4-propylenedioxythiophene)/mno2 composites and their applications in the adsorptive removal of methylene blue

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Progress in Natural Science:Materials International 2016年第1期26卷 32-40页

作者： Ruxangul Jamal Li Zhang Minchao Wang Qin Zhao Tursun Abdiryim Key Laboratory of Petroleum and Gas Fine Chemicals Educational Ministry of China College of Chemistry and Chemical Engineering Xinjiang University Key Laboratory of Functional Polymers Xinjiang University

The poly(3,4-propylenedioxythiophene)/Mn Ocomposites(PPro DOT/Mn O) were prepared successfully by soaking the PPro DOT powders into potassium permanganate(KMn O) solution, with the mass ratio of PPro DOT and KMn Ofrom 2:1 to 1:2. The structure and morphology of composites were characterized by Fourier transform infrared spectroscopy(FTIR), Raman spectroscopy, ultraviolet–visible absorption spectra(UV), X-ray diffraction(XRD), energy-dispersive X-ray spectroscopy(EDX) and field emission scanning electron microscope(FE-SEM).Furthermore, PPro DOT/Mn Ocomposites were tested as the adsorbents for removal of methylene blue(MB) from aqueous solution. The results revealed that the composites were successfully synthesized, and the thiophene sulfur was oxidized into sulfoxide by KMn O. The highest percentage removal of MB after 30 min was 91% for PPro DOT/Mn O(1:2) composite, and the percentage removal of MB was 12 mg g(~-1)after 60 min at initial concentrations of MB dye of 5.6 mg Lin the case of PPro DOT/Mn O(1:2) composite. Besides, the adsorption process of PPro DOT/Mn O(1:2) composite was described by pseudo-second-order and Langmuir models.

关键词： Poly(3,4-propylenedioxythiophene) mno2 Composite Adsorptive removal Methylene blue

Uniform mno2 nanostructures supported on hierar- chically porous carbon as efficient electrocatalysts for rechargeable Li-O2 batteries

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Nano Research 2015年第1期8卷 156-164页

作者： Xiaopeng Han Fangyi Cheng Chengcheng Chen Yuxiang Hu Jun Chen Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) College of Chemistry Collaborative InnovationCenter of Chemical Science and Engineering Nankai University Tianjin 300071 China

直在 situ 氧化还原作用免职和 mno 的生长层次地多孔的碳( HPC )上的 2 nanostructures ， mno 2 /HPC 混血儿为非水的 Li-O 作为阴极催化剂被综合了并且采用 2 节电池。由于温和合成条件， mno 2 一致地在碳支持的表面上被散布... 详细信息

直在 situ 氧化还原作用免职和 mno 的生长层次地多孔的碳( HPC )上的 2 nanostructures ， mno 2 /HPC 混血儿为非水的 Li-O 作为阴极催化剂被综合了并且采用 2 节电池。由于温和合成条件， mno 2 一致地在碳支持的表面上被散布，没有破坏层次多孔的 nanostructure。作为结果，同样准备的 mno 2 /HPC nanocomposite 展出优秀 Li-O 2 电池性能包括低费用过电位，直到 300 的好率能力和长周期稳定性与控制 1,000 mAh

关键词：可充电锂电池二氧化锰纳米结构 mno2 均匀分布多孔碳电催化剂纳米复合材料

Effects of crystal structure on the activity of mno2 nanorods oxidase mimics

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Nano Research 2020年第3期13卷 709-718页

作者： Yanxia Meng Kunfeng Zhao Zhaokun Zhang Peng Gao Jing Yuan Ting Cai Qin Tong Gang Huang Dannong He School of Medical Instrument and Food Engineering University of Shanghai for Science and Technology516 Jungong RoadShanghai200093China School of Materials Science and Engineering Shanghai Jiao Tong University800 Dongchuan RoadShanghai200240China National Engineering Research Center for Nanotechnology 28 East Jiangchuan RoadShanghai200241China Shanghai University of Medicine and Health Sciences 279 Zhouzhu RoadShanghai201318China Ningbo Fundenergy Co. Ltd.699 Haicheng RoadNingbo315200China

The crystal structures would directly affect the physical and chemical properties of the surface of the material,and would thus influence the catalytic activity of the material.α-mno2,β-mno2 andγ-mno2 nanorods with the same morphology yet different crystal structures were prepared and tested as oxidase mimics using 3,3’,5,5’-tetramethylbenzidine(TMB)as the substrate.β-mno2 that exhibited the highest activity had a catalytic constant of 83.75μmol·m^−2·s^−1,2.7 and 19.0 times of those ofα-mno2 andγ-mno2(30.91 and 4.41μmol·m^−2·s^−1),*** characterization results showed that there were more surface hydroxyls as well as more Mn4+on the surface of theβ-mno2 *** surface hydroxyls were conducive to the oxidation reaction,while Mn4+was conducive to the regeneration of surface *** synergistic effect of the two factors significantly improved the activity ofβ-mno2 oxidase ***β-mno2,aβ-mno2-TMB-GSH system was established to detect the content of glutathione(GSH)rapidly and sensitively by *** method had a wide detection range(0.11-45μM)and a low detection limit(0.1μM),and had been successfully applied to GSH quantification in human serum samples.

关键词： crystal phase structure mno2 oxidase mimics surface hydroxyls 3,3’,5,5’-tetramethylbenzidine(TMB) glutathione

Importance of Metal Cations and Water for Stability of mno2 Crystals

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Chinese Journal of Chemical Physics 2015年第6期28卷 -页

作者： Zhi-gang Wei Jia-hong Yan Yang Wu Yue Liu School of Chemical Engineering and Light Industry Guangdong University of Technology Guangzhou 510006 ChinaInstitute of Theoretical Chemistry Jilin University Changchun 130023 China School of Chemical Engineering and Light Industry Guangdong University of Technology Guangzhou 510006 China College of Chemistry Liaoning University Shenyang 110036 China

Metal cations as well as water are important factors to control the synthesis of mno2crystal nanostructures. In this work, systemic Density functional theory calculations about α, β, δ-mno2are presented to show the importance of metal cations and water for the structure stability and energy stability of mno2. It is shown that the α-mno2crystal and its (110) surface will crash without the tunnel cations such as K+, and the distance between the layers of the δ-mno2will be significantly lower than that of the experimental results without the interlayer metal cations and water. At the same time, α-mno2and δ-mno2can be more stable than β-mno2with metal cations and water, and vice versa.

关键词： mno2 Density functional theory Metal cation Formation energy Structure simulation

Dual-modal Colorimetric and Fluorometric Method for Glucose Detection Using mno2 Sheets and Carbon Quantum Dots

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Chemical Research in Chinese Universities 2019年第5期35卷 767-774页

作者： WANG Chengke TAN Rong LI Libo LIU Dong College of Food and Biological Engineering Jiangsu UniversityZhenjiang 212013P.R.China Henan Key Laboratory of Bioniolecular Recognition and Sensing Shangqiu Normal UniversityShangqiu 476000P.R.China School of Agricultural Equipment Engineering Institute of Agricultural EngineeringJiangsu UniversityZhenjiang 212013P.R.China

A novel dual-modal fluorometric and colorimetric method was developed for glucose detection using mno2 sheets and carbon quantum dots(CQDs). The glucose could be oxidized by glucose oxidase, in accompanied witli the fbnnation of H2O2 intennediate, which resulted in the decomposition of mno2 sheets, as well as tlie mno2 sheets(brown) changed to Mn^2+ ions(colorless), which induced the absorption of mno2 sheet decreased and the fluorescence of CQDs increased, consequently. The linear detection ranges of glucose are 5-1000 μmol/L by fluorescent method and 5-60 μmol/L by colorimetric method. The limits of detection of these two measurements are 2.11 and 2.18 μmol/L, respectively. This method is easy to conduct, has reasonable sensitive and selectivity, and could be applied for the glucose detection in real human senim.

关键词： mno2 Carbon quantum dot Colorimetric Fluorescent Dual-modal

Facile synthesis of α-mno2 micronests composed of nanowires and their enhanced adsorption to Congo red

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Frontiers of Chemical Science and Engineering 2014年第1期8卷 64-72页

作者： Weixin ZHANG School of Chemical Engineering Hefei University of Technology Hefei 230009 China Anhui Key Laboratory of Controllable Chemical Reaction & Material Chemical Engineering Hefei 230009 China

In this paper, α-mno2 micronests composed of nanowires were fabricated via a hydrothermal reaction of MnSO4. H20 and K2S208 solutions. The α-mno2 micron- ests were demonstrated to have a higher adsorption capacity than 7-mno2 microspheres due to their large specific surface area. The amount of Congo red adsorbed per unit weight of α-mno2 micronests increased signifi- cantly from 114 to 282mg.g-1 with concentration of Congo red solution increasing from 50 to 200 mg. L-1, but it had a little change with temperature. Kinetics, isotherms and thermodynamics for the adsorption of Congo red on α- mno2 micronests were examined. The adsorption process followed the pseudo-second-order kinetics with good correlation. The experimental data were analyzed by Langmuir and Freundlich models, and equilibrium data fitted the Langmuir isotherm very well with maximum monolayer adsorption capacity of 625 mg. g-1 at 22 ℃. The adsorption was spontaneous and endothermic accord- ing to thermodynamic studies. The experimental results indicate that α-mno2 micronests possess a high adsorption capacity and could be employed as a replacement of traditional sorbents.

关键词： mno2 Congo red adsorption kinetics isotherm thermodynamics

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