生物大分子介导仿生矿化制备磁性纳米粒子的研究进展

doi:10.16085/j.issn.1000-6613.2020-1165

摘要/Abstract

摘要：

相比其他纳米材料，磁铁矿（Fe₃O₄）纳米粒子由于具有磁响应性而被广泛应用于酶固定化、定向给药及核酸提取等方面。不同大小和形状的磁铁矿纳米颗粒可用于不同的领域，如晶体尺寸越小的Fe₃O₄对人体副作用越小，有望用于疾病高效、靶向治疗。近年来，控制Fe₃O₄纳米粒子大小和形貌的新方法研究逐步成为热点。因此，本文回顾了传统的共沉淀制备磁性纳米颗粒的方法，这些方法需要使用有机溶剂或高温等条件控制，介绍了这些方法存在的环境污染和安全性问题。在此基础上，本文深入介绍了近年来出现的一种受自然界生物矿化启发的生物大分子介导的仿生矿化制备磁性纳米粒子的新趋势，综述了生物大分子蛋白质（或多肽）介导的仿生矿化的最新研究进展，阐释了该方法在磁铁矿（Fe₃O₄）纳米粒子的大小和形貌控制方面的优缺点，并对其应用前景及面临的挑战进行了展望。

关键词: 磁性纳米粒子, 多肽, 生物分子工程, 生物模板矿化, 尺寸及形貌控制

Abstract:

Compared with other nanomaterials, Fe₃O₄ nanoparticles are widely used in enzyme immobilization, targeted drug delivery and nucleic acid extraction due to their unique magnetic properties. However, their applications in different aspects have different requirements on the size and morphology of the particles themselves. For example, the smaller Fe₃O₄ has the less side effects to the human body and is more promising for the effective targeted treatment of diseases. The precise control of the size and shape of the magnetite nanoparticles becomes particularly important in recent years. Therefore, this paper reviewed the traditional methods of preparing magnetic nanoparticles by co-precipitation, which require the use of organic solvents or high temperature control, and introduced the environmental pollution and safety problems existing in these methods. Besides, we expounded the new trend of the preparation of magnetic nanoparticles by biological macromolecule mediated biomimetic mineralization which is inspired by biomineralization in nature. Moreover, the latest research progress in protein (or peptide) mediated biomimetic mineralization for the preparation of magnetic nanoparticles was reviewed as well. The advantages and disadvantages of the methods in the size and shape control of magnetite (Fe₃O₄) nanoparticles, together with the challenges were also addressed.

Key words: magnetite nanoparticles, polypeptide, biomolecule engineering, biotemplating mineralization, control of size and morphology

中图分类号:

周雁红, 李夏兰, 张光亚. 生物大分子介导仿生矿化制备磁性纳米粒子的研究进展[J]. 化工进展, 2021, 40(5): 2719-2729.

ZHOU Yanhong, LI Xialan, ZHANG Guangya. Research progress of biomacromolecular-mediated biomimetic mineralization for the preparation of magnetic nanoparticles[J]. Chemical Industry and Engineering Progress, 2021, 40(5): 2719-2729.

图/表 6

参考文献 75

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制备方法	反应条件	产物特点	形态	参考文献
热分解法	高温，需要添加稳定剂，操作复杂	高单分散性，粒径分布很窄，平均尺寸一般小于30nm	由试剂比例、分解温度及熟化时间决定，形态可控，见图1(a)	[12,16]
微乳液法	需要有机复合物，操作复杂	单分散性，粒径分布较窄，平均尺寸一般大于30nm	形态可控，见图1(b)	[13,17]
水热法	高温高压，操作简单	高单分散性，粒径分布很窄，平均尺寸一般大于100nm	形态可控，见图1(c)	[14]
化学沉淀法	操作简单，在空气中反应	粒径分布较均匀，大小可控	由所用盐的种类、反应温度、Fe²⁺/Fe³⁺比例、pH及介质的离子强度决定，形态不易控制，见图1(d)	[15]

制备方法	反应条件	产物特点	形态	参考文献
热分解法	高温，需要添加稳定剂，操作复杂	高单分散性，粒径分布很窄，平均尺寸一般小于30nm	由试剂比例、分解温度及熟化时间决定，形态可控，见图1(a)	[12,16]
微乳液法	需要有机复合物，操作复杂	单分散性，粒径分布较窄，平均尺寸一般大于30nm	形态可控，见图1(b)	[13,17]
水热法	高温高压，操作简单	高单分散性，粒径分布很窄，平均尺寸一般大于100nm	形态可控，见图1(c)	[14]
化学沉淀法	操作简单，在空气中反应	粒径分布较均匀，大小可控	由所用盐的种类、反应温度、Fe²⁺/Fe³⁺比例、pH及介质的离子强度决定，形态不易控制，见图1(d)	[15]

蛋白名称	结构特点	氨基酸组成	作用	参考文献
Mms6	小分子膜蛋白（12500, pI 4.5），包括一个跨膜螺旋，如图2(a)	主要由一个N端疏水区和含有多个酸性氨基酸的C端亲水区组成。C末端区域含有紧密的羧基和羟基，与铁离子结合。这些蛋白质N端具有共同的序列LGLGLGAWGPXXLGXXGXAGA。此外，中间和C端之间的区域含有一些共同的氨基酸，如赖氨酸（Lys）、酪氨酸（Tyr）和精氨酸（Arg）	定位于磁小体，只存在于趋磁细菌中，与细菌磁铁矿晶体紧密结合。可以与铁离子结合，在成核和磁铁矿晶体生长过程中具有重要作用。其中，以重组蛋白形式表达的MamC和MamD会影响磁铁矿晶体的尺寸，缺失MamC和MamD会导致磁铁矿晶体尺寸的适度减小。	[36,38]
MamC(Mms13)	小分子膜蛋白(12400， pI 7.2)有两个跨膜螺旋，由一个长度为21个残基的小肽连接，如图2(b)			[8,10,37,39]
MamD(Mms7)	小分子膜蛋白，7000,pI 5.9，如图2(c)			[36-37]
MamG(Mms5)	小分子膜蛋白，5000,pI 6.1，如图2(d)			[36-37]
MmsF	MmsF包括3个跨膜螺旋，N端在细胞质中，而C端面对磁小体，如图2(e)	磁小体内的环（C端和第一和第二螺旋之间的环）含有高度保守的残基	除MmsF会导致产生更小且畸形的磁小体，在控制形态方面至关重要。MmsF中的环状结构可以介导MmsF与矿物质或其他生物矿化蛋白的相互作用	[40,43,47]
Mms16（BMP膜特异性GTP酶）	—	—	BMP膜特异性Mms16启动细胞质膜的内陷，形成细胞内囊泡	[37]

蛋白名称	结构特点	氨基酸组成	作用	参考文献
Mms6	小分子膜蛋白（12500, pI 4.5），包括一个跨膜螺旋，如图2(a)	主要由一个N端疏水区和含有多个酸性氨基酸的C端亲水区组成。C末端区域含有紧密的羧基和羟基，与铁离子结合。这些蛋白质N端具有共同的序列LGLGLGAWGPXXLGXXGXAGA。此外，中间和C端之间的区域含有一些共同的氨基酸，如赖氨酸（Lys）、酪氨酸（Tyr）和精氨酸（Arg）	定位于磁小体，只存在于趋磁细菌中，与细菌磁铁矿晶体紧密结合。可以与铁离子结合，在成核和磁铁矿晶体生长过程中具有重要作用。其中，以重组蛋白形式表达的MamC和MamD会影响磁铁矿晶体的尺寸，缺失MamC和MamD会导致磁铁矿晶体尺寸的适度减小。	[36,38]
MamC(Mms13)	小分子膜蛋白(12400， pI 7.2)有两个跨膜螺旋，由一个长度为21个残基的小肽连接，如图2(b)			[8,10,37,39]
MamD(Mms7)	小分子膜蛋白，7000,pI 5.9，如图2(c)			[36-37]
MamG(Mms5)	小分子膜蛋白，5000,pI 6.1，如图2(d)			[36-37]
MmsF	MmsF包括3个跨膜螺旋，N端在细胞质中，而C端面对磁小体，如图2(e)	磁小体内的环（C端和第一和第二螺旋之间的环）含有高度保守的残基	除MmsF会导致产生更小且畸形的磁小体，在控制形态方面至关重要。MmsF中的环状结构可以介导MmsF与矿物质或其他生物矿化蛋白的相互作用	[40,43,47]
Mms16（BMP膜特异性GTP酶）	—	—	BMP膜特异性Mms16启动细胞质膜的内陷，形成细胞内囊泡	[37]

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