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化学进展 2020, Vol. 32 Issue (2/3): 230-238 DOI: 10.7536/PC190620 前一篇   后一篇

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功能性纤维状二氧化硅纳米粒子的调控制备及在吸附分离中的应用

黄倩文1,2, 张晓文2, 李密2, 吴晓燕2, 袁立永1,**()   

  1. 1. 中国科学院高能物理研究所 北京 100049
    2. 南华大学 资源环境与安全工程学院 衡阳 421001
  • 收稿日期:2019-06-20 出版日期:2020-02-15 发布日期:2019-12-19
  • 通讯作者: 袁立永
  • 基金资助:
    国家自然科学基金项目(21777161); 国家自然科学基金项目(21471153); 科学挑战计划(TZ2016004); 南华大学“双一流”建设项目(2019SYL05); 中国科学院青年创新促进会(2017020)
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Preparation of Functional Fibrous Silica Nanoparticles and Their Applications in Adsorption and Separation

Qianwen Huang1,2, Xiaowen Zhang2, Mi Li2, Xiaoyan Wu2, Liyong Yuan1,**()   

  1. 1. Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
    2. School of Resource Environment and Safety Engineering, University of South China, Hengyang 421001, China
  • Received:2019-06-20 Online:2020-02-15 Published:2019-12-19
  • Contact: Liyong Yuan
  • About author:
    ** e-mail:
  • Supported by:
    National Natural Science Foundation of China(21777161); National Natural Science Foundation of China(21471153); Science Challenge Project(TZ2016004); Double First Class Construct Program of University of South China(2019SYL05); Youth Innovation Promotion Association, CAS(2017020)

利用吸附剂对环境中污染物进行分离去除是环境污染治理的有效方法和常用方法,其中以无机材料为载体的功能化吸附剂应用更为广泛。二氧化硅纳米颗粒具有稳定性好、易修饰、成本低和对环境友好等特点,在环境污染物的吸附分离方面具有广阔的应用前景。纤维状硅球与传统的二氧化硅纳米颗粒相比具有比表面积大、有开放孔道等优点,在实际吸附分离应用中能够提供更多有效吸附位点且孔道不易堵塞,是一种更具潜力的吸附剂载体。本文结合本课题组的研究工作对纤维状硅球的合成制备尤其是结构参数的调控方面进行了归纳分析;在分析近年来关于重金属、有机物、放射性核素等环境污染物处理相关研究的基础上,对功能性纤维状硅球在环境污染物吸附分离领域中的应用进行总结;最后从纤维状硅球合成方面的局限性以及应用方面的潜力对功能性纤维状硅球在吸附分离领域中的应用前景进行了展望。

关键词： 纤维状二氧化硅, 功能化, 形貌调控, 吸附, 放射性核素

The use of solid adsorbents to separate and remove pollutants from the environment is an effective and common method for environmental pollution control, in which functional adsorbents based on inorganic materials are more widely used. Silica nanoparticles feature good stability, easy modification, low cost and environmental friendliness, thus leading to widespread potential in the treatment of environmental pollutants. Compared with traditional silica nanoparticles, fibrous silica spheres have the advantages of large specific surface area and open pores, which can provide more effective adsorption sites and ensure that pore channels are not easily blocked during practical applications, and thus show more potential in adsorption applications. In this paper, the synthesis and preparation of fibrous silica spheres, in particular, the regulation of structural parameters, are summarized and analyzed based on the reported researches and the works of our group. The application of functional fibrous silica spheres in the adsorption and separation of environmental pollutants in recent years is then reviewed and summarized following the analysis of recent progress in the treatment of heavy metals, organics, radionuclides and other environmental pollutants. Finally, the application of functional fibrous silicon sphere in the field of adsorption and separation is prospected from the points of view of limitations of fiber-like silicon sphere synthesis and application potentials.

Key words: fibrous silica, functionalization, morphology control, adsorption, radionuclide
()
图1 DFNS经典合成路径[3]
Fig.1 The classical synthesis path of DFNS[3]
图2 树枝状纤维形纳米硅球的SEM(左)和TEM(右)图[3]
Fig.2 SEM(left) and TEM(right) imgaes of dendritic fibrous nanosilica[3]
图3 裹挟DFNS的微乳液电子显微镜(SEM)照片
Fig.3 SEM image of microemulsion with DFNS
表1 DFNS结构参数的影响因素分析
Table 1 Analysis of influencing factors of DFNS structure parameters
Factors Influence ref
Template
(CPB etc)		 Template with different alkyl chain lengths can adjust the particle size of DFNS; Increasing the amount of template can hinder the nucleation reaction at the initial stage and thus reduce the particle size; The molar ratio of the template and silicon can affect the particle size and the shape of the pore wall, but there is no specific research conclusion on the influence trend. 31, 33~36
Silicon hydrolyzer
(urea etc)		 Urea is used to hydrolyze silicon reagent, which can be hydrolyzed at room temperature. Before heating reaction, the more urea content, the longer stirring time, the more nucleated particles and the smaller DFNS particle size. 34
Auxiliary organic solvent
(pentanol etc)		 Increasing the alkyl chain length of the auxiliary organic solvent can increase the fold spacing.Reducing its dosage can increase homogeneity, reduce particle size and fold interval.The use of alcohols of different polarity, such as n-propanol and n-octanol, can regulate particle size. 34, 37, 38
Organic solvent
(cyclohexane etc)		 As the amount of organic solvent increases, the particle size decreases, the homogeneity of particles and the pore size increase, and the channel form finally becomes folded. As the polarity of solvent increases, the particle size first increases and then decreases. 33, 34, 37, 39
Silicon original reagent
(TEOS etc)		 As the amount of silicon reagent increases, the fiber density increases, the specific surface area and the particle size decreases. 36, 39, 40
Stir speed during
growing period		 With the increase of stirring speed, the particle size becomes smaller and the pore size becomes larger. 41
Growth reaction
temperature		 With the increase of reaction temperature,the homogeneity of particles and the particle size increase, the fiber density, the specific surface area, the pore capacity and the pore diameter decrease. 34, 41
Growth reaction time With the increase of reaction time, the homogeneity of particles, the particle size, the fiber density and the pore size all decreased. 34, 37~39
图4 种子生长法合成DFNS[42]
Fig.4 Synthesis of DFNS by seed growth method[42]
图5 特殊结构DFNS的纳米粒子TEM图(a, b)不对称羽毛球形核壳结构[26];(c, d)蛋黄-蛋壳三层核壳结构[47]
Fig.5 TEM images of special DFNS structure nanoparticles,(a,b) asymmetric shuttlecock core-shell structure[26];(c,d) yolk-shell three-layer core-shell structure[47]
表2 多种形貌硅基吸附材料的吸附效果对比
Table 2 Comparison of adsorption ability among silicon-based adsorption materials of various morphologies
Morphology Adsorbents Adsorbate Adsorption capacities(mg·g-1) Equilibration time(min) ref
MCM-41 MCM-41-AO U(Ⅵ) 384.59 720 54
KIT-6 KIT-6-AO U(Ⅵ) 323.94 45 55
Nanosheet ImP(O)(OH)2/SiO2 U(Ⅵ) 618 60 56
SBA-15 AO@SBA-15 U(Ⅵ) 625 30 57
SBA-15 U(Ⅵ) 235 30 58
DFNS F-SiO2-DP U(Ⅵ) 416 10 59
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