树枝状纤维形二氧化硅纳米粒子的研究进展

doi:10.15541/jim20180247

无机材料学报 ›› 2018, Vol. 33 ›› Issue (12): 1274-1288.DOI: 10.15541/jim20180247

所属专题：药物载体与防护材料

树枝状纤维形二氧化硅纳米粒子的研究进展

王亚斌¹, 刘忠^2,3, 史时辉¹, 呼科科¹, 张琰图¹, 郭敏^2,3

1. 延安大学化学与化工学院, 延安 716000;
2. 中国科学院青海盐湖研究所, 中国科学院盐湖资源综合高效利用重点实验室, 西宁 810008;
3. 青海省盐湖资源化学重点实验室, 西宁 810008

收稿日期:2018-05-29 修回日期:2018-06-29 出版日期:2018-12-20 网络出版日期:2018-11-27
作者简介:王亚斌(1985-), 男, 博士, 讲师. E-mail: ybw@yau.edu.cn
基金资助:
国家自然科学基金(U1607105);中国科学院青年促进会项目(2016377);陕西省自然科学基金(2016ZDJC-19);延安大学博士科研启动项目(YDBK2017-39, YDBK2016-14);青海省科技项目(2018-GX-101, 2018-ZJ-722)

Research Progress of Dendritic Fibrous Nano-silica (DFNS)

WANG Ya-Bin¹, LIU Zhong^2,3, SHI Shi-Hui¹, HU Ke-Ke¹, ZHANG Yan-Tu¹, GUO Min^2,3

1. College of Chemistry and Chemical Engineering, Yan’an University, Yan’an 716000, China;
2. Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining 810008, China;
3. Key Laboratory of Salt Lake Resources Chemistry of Qinghai Province, Xining 810008, China

Received:2018-05-29 Revised:2018-06-29 Published:2018-12-20 Online:2018-11-27
About author:WANG Ya-Bin. E-mail: ybw@yau.edu.cn
Supported by:
National Natural Science Foundation of China (U1607105);Youth Innovation Promotion Association (2016377);Natural Science Foundation of Shaanxi Province (2016ZDJC-19);Doctoral Research Program of Yan’an University (YDBK2017-39, YDBK2016-14);Science and Technology Funding in Qinghai Province (2018-GX-101, 2018-ZJ-722)

摘要/Abstract

摘要：

与传统二氧化硅介孔材料相比, 树枝状纤维形二氧化硅纳米粒子(Dendritic Fibrous Nano-silica, DFNS), 特别是具备三维中心辐射状孔道和多级孔结构的球形DFNS拥有较高的比表面积、较大的孔体积、较高的孔渗透性和粒子内表面更易接触性等优点。客体物质(如极小的纳米粒子)能够沿着中心辐射状孔道进行负载和/或输送, 甚至与化学改性所得内部活性位点发生反应。因此, DFNS是一种富有前景的载体平台, 可以用来构筑新型纳米催化剂、吸附剂、基因/蛋白质/药物的递送系统等。大量研究表明: 球形DFNS与生俱来的结构优势使其能够作为MCM-41和SBA-15的理想替代材料。但是, DFNS领域依旧存在很多需要探讨的问题。因此, 本文主要归纳分析DFNS的结构特征、常用结构模型、新型结构和实时应用。希望能够给予材料和化学科学家一些参考, 促进DFNS的蓬勃发展。

关键词: 树枝状纤维形, 二氧化硅, 结构模型, 新颖结构, 实时应用

Abstract:

Dendritic fibrous nano-silica (DFNS), especially the sphere-shaped with three-dimensional (3D) center- radial channels and hierarchical pores, possess higher specific surface areas, larger pore volumes, higher pore permeability, more accessible internal spaces, etc. Guest substances (e.g., ultrasmall nanoparticles) can be loaded onto and transported in the radial nanochannels, or can even react with the chemically active sites in these nanochannels. As a result, DFNS can serve as promising platforms to construct novel nanocatalysts, adsorbent materials, and delivery systems for genes, proteins or drugs. A majority of investigations about DFNS have demonstrated that silica nanospheres with this special topography have inherent superiorities over traditional mesoporous MCM-41 or SBA-15, and can be perfect alternatives. Nevertheless, reviews on DFNS are limited, and there still exist plenty of issues that need to be probed into. Therefore, this comprehensive review provides a critical survey on DFNS’ structural characteristics, commonly used structural models, novel structures, real-time applications, etc. We sincerely expect that this paper could give material scientists and chemists certain inspiration to accelerate DFNS family’s booming evolution.

Key words: dendritic fibrous, silica, structural models, novel structures, real-time applications

中图分类号:

O611
TB383

王亚斌, 刘忠, 史时辉, 呼科科, 张琰图, 郭敏. 树枝状纤维形二氧化硅纳米粒子的研究进展[J]. 无机材料学报, 2018, 33(12): 1274-1288.

WANG Ya-Bin, LIU Zhong, SHI Shi-Hui, HU Ke-Ke, ZHANG Yan-Tu, GUO Min. Research Progress of Dendritic Fibrous Nano-silica (DFNS)[J]. Journal of Inorganic Materials, 2018, 33(12): 1274-1288.

图/表 9

图1 树枝状纤维形二氧化硅纳米球的透射电镜(a)~(c)和扫描电镜(d)~(f)照片[23]

Fig. 1 TEM (a-c) and SEM (d-f) images of silica-based nanospheres with dendritic fibrous morphologies[23]

表1 树枝状纤维形二氧化硅纳米粒子称谓概括

Table 1 English and Chinese appellations, and their abbreviations for silica nanoparticles with dendritic fibrous structures

No.	English appellation	Appellation abbreviation	Chinese appellation	Ref.
1	Dendritic fibrous nanosilica	DFNS or (KCC-1)	树枝状纤维形二氧化硅纳米粒子	[25-28, 30]
2	Three dimensional dendritic mesoporous silica nanospheres	3D dendritic MSNSs	三维树枝状介孔二氧化硅纳米球	[22, 31-32]
3	Dendrimer-like silica nanoparticles with hierarchical pores	HPSNs	树枝状多级孔二氧化硅纳米粒子	[17,21,33-34]
4	Dendritic mesoporous silica nanoparticles	DMSNs	树枝状介孔二氧化硅纳米粒子	[35-42]
5	Dendritic mesoporous silica nanospheres	DMSNs	树枝状介孔二氧化硅纳米球	[43-45]
6	Fibrous mesoporous silica microspheres	FMSMs	纤维形介孔二氧化硅微球	[46-47]
7	Wrinkled silica nanoparticles	WSNs	褶皱状二氧化硅纳米粒子	[48-52]
8	Wrinkled mesoporous silica	WMS	褶皱状介孔二氧化硅	[53-56]
9	Wrinkled mesoporous silica nanoparticles	WMSNs	褶皱状介孔二氧化硅纳米粒子	[57-58]
10	Radial-like mesoporous silica	RMS	中心辐射状介孔二氧化硅	[59-60]
11	Fibrous silicon dioxides spheres	FSS	纤维形二氧化硅球	[61]
12	Fibrous silica nanoparticles or nanospheres	FSNs	纤维形二氧化硅纳米粒子或纳米球	[62]
13	Hierarchically and radially mesoporous silica	HRM	分层次和辐射状介孔二氧化硅	[63]
14	Hierarchically structured spherical mesoporous nanoflowers	HSMNF	分层次结构球形介孔纳米花”和	[64]
15	Mesostructured silica nanoparticles	MSNs	介孔结构二氧化硅纳米粒子	[33, 65-67]
16	“Dendritic”	-		[13, 68-70]
17	“Fibrous”	-		[71-79]

图2 树枝状纤维形二氧化硅纳米球的结构态转变[89]

Fig. 2 The structural transformation of a DFNS from a quasi dendritic state[89] (a) to a quasi radially fibrous state[23] (c) through an intermediate state of “dendritic fibrous”[11] (b). The forming process of a dendrimer by iterative grafting steps (d)

图3 DFNS相关文献逐年发表情况(a)及应用领域范围(b)

Fig. 3 The percentages of published literatures about DFNS from 2008 to 2018 (a), and the percentages of various applications for DFNS (b)

图4 球形DFNS常用结构模型

Fig. 4 The commonly used morphological models for DFNS spheres.

图5 不同结构二氧化硅纳米粒子的二维示意图[110,127,149-150]

Fig. 5 Schematic diagrams of 2D planar structures from various silica nanospheres[110,127,149-150] (a) DFNS; (b) Hierarchical radial porous sphere; (c) Hierarchical porous sphere; (d) Radial porous sphere with a magnetic core; (e) Porous sphere with a magnetic core; (f) Sunflower-like magnetic porous sphere

表2 KCC-1环己烷乳液法、乙醚乳液法和油水双相分层法适用性对比

Table 2 Comparison of the approaches applied to synthesize DFNS spheres, including: cyclohexane emulsions for KCC-1, ethyl ether emulsion for HSMNs, and biphase stratification technique for 3D dendritic MSNSs

Synthetic approach	Cyclohexane emulsions for DFNS or KCC-1	Ethyl ether emulsion for HSMNs	Biphase stratification for 3D dendritic MSNSs
Pore size range	ca. 2-30 nm	ca. 8-200 nm	ca. 2.8-10 nm
Particle size range	ca. 170-1120 nm	ca. 100-1100 nm	ca. 180-280 nm
Repeatability	Excellent	Excellent	Excellent
Maneuverability	Easy	Easy	Normal
Particles’uniformity	Poor	Poor	Excellent
Pores’ uniformity	Good	Average	Excellent
By-product	None	Some	None
Intermediate products	Some	Some	None
Universality	~70%	~17%	~3%
Significance	Facility and universality	Macropores for diverse guests	Uniformity for fine control

图6 不同结构DFNS类复合纳米粒子的TEM照片

Fig. 6 TEM images of nanoparticles with diverse morphologies developed by means of DFNS reaction systems(a) Core-shelled Fe3O4@SiO2@KCC-1[8]; (b) Fe3O4/DFNS composites[47]; (c) Core-shelled TS-1@KCC-1[80]; (d) Core-shelled SiO2@DFNS[134]; (e) Hollow DFNS [86]; (f) Janus DFNS/Mg@Au[121]; (g) Shuttlecock-shaped DFNS Au@Mg-DFNS[48]; (h) Yolk-shelled Fe3O4@DFNS[144]; (i) Yolk-shelled DFNS/Pt@MSS[159]

图7 树枝状纤维形纳米粒子的设计合成、结构设计以及应用前景示意图

Fig. 7 Schematic illustration of designed synthesis, designed structures, and promising applications for dendritic fibrous nano-particles

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树枝状纤维形二氧化硅纳米粒子的研究进展

Research Progress of Dendritic Fibrous Nano-silica (DFNS)

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