CN111436454A - 金属有机骨架材料的抗病毒用途 - Google Patents
金属有机骨架材料的抗病毒用途 Download PDFInfo
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- A01N37/44—Biocides, pest repellants or attractants, or plant growth regulators containing organic compounds containing a carbon atom having three bonds to hetero atoms with at the most two bonds to halogen, e.g. carboxylic acids containing at least one carboxylic group or a thio analogue, or a derivative thereof, and a nitrogen atom attached to the same carbon skeleton by a single or double bond, this nitrogen atom not being a member of a derivative or of a thio analogue of a carboxylic group, e.g. amino-carboxylic acids
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- A01N43/00—Biocides, pest repellants or attractants, or plant growth regulators containing heterocyclic compounds
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Abstract
本发明涉及非医药领域，提供了金属有机骨架材料抗病毒的新用途。通过使病毒与金属有机骨架材料在光照条件下接触，能够快速、高效得得到优良的抗病毒效果。金属有机骨架材料由金属源及有机配体作用形成。
Description
技术领域
本发明属于非医药领域，具体涉及一种使用金属有机骨架材料的抗病毒用途及抗病毒装置。
背景技术
病毒是由一个核酸分子(DNA或RNA)与蛋白质构成的非细胞形态，靠寄生生活的介于生命体及非生命体之间的有机物种。病毒可以感染几乎所有具有细胞结构的生命体，对人体健康产生严重危害。现在环境污染情况不容乐观，央视《走进科学》栏目曾经报道，雾霾天气下，PM2.5中携带有大量的细菌、真菌和DNA病毒，最低估计有1300多种。在现在污染环境条件下，医院、学校、单位、家庭等所有人类聚集活动场所，杀灭环境中的一些病毒，显得尤为重要。
目前杀灭环境中的方法有消毒剂，例如醛类、含氯消毒剂、酚类、氧化剂、碱类等消毒剂，高温蒸煮等方法。但是现有的消毒方法仍然存在一些不尽如人意的地方，例如消毒剂难耐的气味、化学物质对人体的影响、操作不便等。
金属有机骨架是一类多孔材料，由金属源（例如金属团簇、金属氧化物或金属盐等）与有机配体作用形成具有周期性网络结构的有机无机杂化材料，具有孔隙率高、官能团丰富、孔道有序、结构多样等众多优点，目前该新型功能性材料在气体储存与分离、催化、膜、传感、生物医学成像等领域发挥着重要作用。
发明内容
本发明提供了金属有机骨架材料抗病毒的新用途，使病毒与金属有机骨架材料在光照条件下接触，所述金属有机骨架材料由金属源及有机配体作用形成。
优选地，所述病毒包括H1N1流感病毒、肠道病毒EV71。
优选地，所述金属源中的金属元素选自Cu、Zn、Zr中的至少一种。
优选地，所述有机配体选自均苯三酸、2-氨基对苯二甲酸、2-甲基咪唑、苯并咪唑中的至少一种。
本发明还提供一种抗病毒装置，包括金属有机骨架材料和光源，所述金属有机骨架材料由金属源及有机配体作用形成。
优选地，金属源中的金属元素选自Cu、Zn、Zr中的至少一种。
优选地，所述有机配体选自均苯三酸、2-氨基对苯二甲酸、2-甲基咪唑、苯并咪唑中的至少一种。
通过使用金属有机骨架材料进行抗病毒，能够有效杀灭非人体环境中的病毒。并且，不会存在难耐的气味等问题、操作简便。
附图说明
附图是用来提供对本发明的进一步理解，并且构成说明书的一部分，与下面的具体实施方式一起用于解释本发明，但并不构成对本发明的限制。
图1为抗病毒的示意图；
图2为实施例1-4所用的金属有机骨架材料的X射线衍射图谱，其中图2A为实施例1所用的金属有机骨架材料的X射线衍射图谱，图2B为实施例2所用的金属有机骨架材料的X射线衍射图谱，图2C为实施例3所用的金属有机骨架材料的X射线衍射图谱，图2D为实施例4所用的金属有机骨架材料的X射线衍射图谱。
具体实施方式
以下结合附图对本发明的具体实施方式进行详细说明。应当理解的是，此处所描述的具体实施方式仅用于说明和解释本发明，并不用于限制本发明。
本发明所使用的术语等为本领域通常具有的含义，以下对本发明所使用的一些技术术语进行解释及定义。
“抗病毒”一般指的是采用化学或物理方法杀灭病毒或妨碍病毒生长繁殖及其活性的过程。在本发明中，尤其指的是活性病毒的浓度在与金属有机骨架材料接触后，与在金属有机骨架材料接触前相比，具有明显降低。
本发明所使用的“金属有机骨架材料”，金属有机骨架是一类功能多孔材料，由金属源（例如金属团簇、金属氧化物或金属盐等）与有机配体通过配位作用构筑而成，兼具无机和有机孔材料的优点，具有比表面积高、孔道有序可重复、官能团丰富、稳定性好、结构多样等特点。本发明使用的金属有机骨架材料可以使用本领域已知的方法合成，例如水热法、搅拌静置法、电解法、纺丝法、微波法、热压法等。上述合成方法例如记载于Katz, M. J. et al. A facile synthesis of UiO-66, UiO-67 and their derivatives. Chem. Commun.49, 9449-9451, (2013)；Park, K. S. et al. Exceptional chemical andthermal stability of zeolitic imidazolate frameworks. P. Natl. Acad. Sci. U S A.103, 10186-10191, (2006)；Li S. et al.Creating Lithium-Ion Electrolytes withBiominmetic Ionic Channels in Metal-Organic Frameworks. DOI: 10.1002/adma.201707476.等文献中。不同的合成方法制备的金属有机骨架材料均可用于杀灭病毒，其中，热压法是本申请的发明人首创的方法，其记载于中国专利ZL201510630401.X，上述专利或文献全文引入本发明。
本发明中的“光照条件”可以为自然光或人造光等，只要能够激发金属有机骨架材料产生光生电子和光生空穴即可，没有特别限制。本发明下述的实施例中以荧光灯为例，其中色温5000K，光照强度1400lx，光照时间1小时。
下面对本发明的抗病毒用途进行详细说明。
本发明公开了金属有机骨架材料的抗病毒用途，使病毒与金属有机骨架材料在光照条件下接触，其中金属有机骨架材料由金属源及有机配体作用形成。
金属有机骨架材料可能通过以下两种方式在光照条件下杀灭病毒：第一，直接接触式使病毒失活，金属有机骨架材料在光照的条件下，产生光生电子和光生空穴，光生电子和光致空穴直接破坏病毒的组成成分，导致功能单元失活而使病毒死亡。第二，光激发催化剂与病毒间的间接反应，即光生电子或光生空穴与水、水中的溶解氧以及空气中的氧反应，形成超氧自由基(•O2 ‒)、过氧化氢(H2O2)和羟基自由基(•OH)等活性氧类物质。以实施例1为例说明，在大于其带隙能的光照条件下，电子就可以从价带激发到导带，同时价带产生相应的空穴，但存在合适的捕获剂时，电子和空穴的复合受到抑制，就可以在材料表面发生氧化还原反应，生成活性羟基、超氧离子、过羟基和双氧水等，这些都可与生物大分子如脂类、蛋白质、酶类以及核酸大分子反应，直接损害或通过一系列氧化链式反应对生物大分子造成广泛的损伤性破坏。
金属有机骨架材料可以用于各种常见病毒，例如H1N1流感病毒、肠道病毒EV71、噬菌体、肝炎病毒HAV、轮状病毒、麻疹病毒、肝炎病毒等。以下实施例以H1N1流感病毒、肠道病毒EV71为例进行说明。
关于金属有机骨架材料，其由金属源及有机配体作用形成。本领域技术人员可以使用已知的、如本发明上文所述的方法合成金属有机骨架材料，上述方法合成的金属有机骨架材料在光照条件下均具有卓越的抗病毒效果。
本发明的金属有机骨架材料的金属源可以为金属团簇、金属氧化物、金属离子等，金属源中包含的金属元素可以自由选择，例如为Mg、Sc、Y、Ti、Zr、V、Nb、Cr、Mo、Mn、Fe、Ru、Co、Rh、Ni、Cu、Zn、Cd、Al、Ga、In、Ce、Nd、Sm、Gd、Er、Si中的至少一种。优选地，金属元素包含Cu、Zn、Zr中的至少一种。当金属元素为Cu、Zn、Zr中的至少一种时，得到的金属有机骨架材料的抗病毒效果优良，达到90%以上。有机配体可以为含氧、氮等的多齿有机配体，例如均苯三酸、2-氨基对苯二甲酸、2-甲基咪唑、苯并咪唑等。
在本发明中，所制备的金属有机骨架材料通过X射线粉末衍射进行表征，其中使用的仪器为Bruker D8 Advance（布鲁克，德国），参数为电压40Kv、电流15mA、Cu靶，λ＝0.154nm
本发明的发明人发现，与无光条件相比，金属有机骨架材料在光照条件下具有显著的抗病毒效果。金属有机骨架材料对光照条件没有特别的要求，可以根据抗病毒的实际需求优化光照时间、金属有机骨架材料的用量等参数。优选地，使病毒与金属有机骨架材料在光照条件下接触10分钟以上，抗病毒效果更优。
以下实施例1-16评估了金属有机骨架材料的抗病毒效果。其中，光照时间为1小时、光照强度1400lx、金属有机骨架材料的用量为50毫克。实施例1-2使用的病毒为H1NI流感病毒，实施例3-4使用的病毒为肠道病毒EV71。
实施例1
在添加10%血清、2mM L-谷氨酰胺和1mM抗生素的MEM培养基（ Sigma－Aldrich，M2279）上培养MDCK犬肾细胞（ ATCC，型号：NBL－2）。在37℃条件下，流感病毒株A/PR8/34(H1N1)在MDCK细胞上传代3天。MDCK细胞在零下80℃保存，用来测定病毒滴度。对于感染，如图1所示，将顺序稀释的105 TCID50/mL的病毒逐滴均匀滴涂在负载有金属有机骨架材料1的基材2表面上进行处理，并暴露于荧光灯（色温5000K，光照强度1400lx）下1小时。然后将处理后的病毒加入含有80%融合MDCK细胞的96孔板中，在37℃用5%CO2在培养箱中孵育，感染后3天收集上清液进行病毒滴定。此外，进行光空白对照组实验，即为在相同光照条件下使用不添加金属有机骨架材料的空白基材。
抗病毒效果由杀灭率表示，杀灭率根据以下公式进行计算：
Mv=-lg(C/C0)=-[lg(C)-lg(C0)]；
杀灭率=[1-10-Mv]×100%
其中Mv是抗病毒功效值；
C0代表与空白基材接触一定光照时间的病毒液的TCID50/mL；
C代表接触金属有机骨架材料一定光照时间的病毒液的TCID50/mL。
用于负载金属有机骨架材料的基材可以为常见的基材，例如无纺布、真丝布、玻纤、金属网、泡沫金属、聚氨酯海绵、三聚氰胺海绵等，在本实施例中以无纺布为例。
金属有机骨架材料的金属源为硝酸铜、有机配体为均苯三甲酸。制备的金属有机骨架材料的X射线衍射图谱如图2A所示，其中3表示模拟曲线，4表示实验曲线。如图所示，制备的金属有机骨架材料与模拟曲线吻合，说明成功得到了金属有机骨架材料。
实施例2
除了金属有机骨架材料的金属源为四水合硝酸锌、有机配体为2-甲基咪唑，其他与实施例1相同。制备的金属有机骨架材料的X射线衍射图谱如图2B所示，其中5表示模拟曲线，6表示实验曲线。如图所示，制备的金属有机骨架材料与模拟曲线吻合，说明成功得到了金属有机骨架材料。
实施例3
除了金属有机骨架材料的金属源为四氯化锆、有机配体为2-氨基对苯二甲酸、使用的病毒为肠道病毒EV71外，其他与实施例1相同。制备的金属有机骨架材料的X射线衍射图谱如图2C所示，其中7表示模拟曲线，8表示实验曲线。如图所示，制备的金属有机骨架材料与模拟曲线吻合，说明成功得到了金属有机骨架材料。
实施例4
除了金属有机骨架材料的金属源为四水合硝酸锌、有机配体为苯并咪唑。使用的病毒为肠道病毒EV71外，其他与实施例1相同。制备的金属有机骨架材料的X射线衍射图谱如图2D所示，其中9表示模拟曲线，10表示实验曲线。如图所示，制备的金属有机骨架材料与模拟曲线吻合，说明成功得到了金属有机骨架材料。
上述实施例1-4所使用的金属有机骨架材料、病毒以及抗病毒效果记录于表1中。
表1
通过以上实施例及空白对照组可以看出，金属有机骨架材料在光照条件下具有突出的抗病毒效果。
Claims (7)
1.金属有机骨架材料抗病毒用途，其中使病毒与金属有机骨架材料在光照条件下接触，所述金属有机骨架材料由金属源及有机配体作用形成。
2.根据权利要求1所述的用途，其特征在于，所述病毒包括HIN1流感病毒、肠道病毒EV71。
3.根据权利要求1或2所述的用途，其特征在于，所述金属源中的金属元素选自Cu、Zn、Zr中的至少一种。
4.根据权利要求1或2所述的用途，其特征在于，所述有机配体选自均苯三酸、2-氨基对苯二甲酸、2-甲基咪唑、苯并咪唑中的至少一种。
5.一种抗病毒装置，其特征在于，包括金属有机骨架材料和光源，所述金属有机骨架材料由金属源及有机配体作用形成。
6.根据权利要求5所述的装置，其特征在于，所述金属源中的金属元素选自Cu、Zn、Zr中的至少一种。
7.根据权利要求5所述的装置，其特征在于，所述有机配体选自均苯三酸、2-氨基对苯二甲酸、2-甲基咪唑、苯并咪唑中的至少一种。
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