功能化二氧化硅纳米颗粒介电泳行为及其对细胞介电性质影响的研究
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摘要
精确可控和可逆的微米或纳米结构自组装在微纳生化传感领域有着巨大的应用前景,是近年来纳米研究领域的一个热点。介电泳技术是一种很有潜力的纳米操控技术,可以实现纳米颗粒在微电极上的排布及自组装等操作。但是通过介电泳对组装的微纳结构进行精确控制目前仍存在比较大的困难。本论文以功能化二氧化硅纳米颗粒的介电泳行为及其对细胞介电性质的影响为研究目标,通过在二氧化硅纳米颗粒表面修饰磷酸功能基团实现了其在微电极上自组装结构的精确可控和可逆。并且发现功能化二氧化硅纳米颗粒被细胞吞噬后会对其介电性质产生影响。本论文的主要工作包括以下三个方面：
1、不同功能基团修饰对二氧化硅纳米颗粒介电泳自组装行为的影响研究
通过对二氧化硅纳米颗粒、羧基化二氧化硅纳米颗粒、磷酸化二氧化硅纳米颗粒、PEG化二氧化硅纳米颗粒和氨基化二氧化硅纳米颗粒在交流电场下的介电泳自组装行为进行考察,发现带较强负电荷的功能化基团修饰可以有效地增强二氧化硅纳米颗粒在微电极上的自组装行为。其原因是带较强负电荷的功能化基团能增强二氧化硅纳米颗粒表面的阳离子扩散层,从而提高其表面电导率。这为有针对性地改善纳米颗粒在水溶液中的介电性质,使其更好进行介电泳白组装提供了有力的实验依据。
2、基于介电泳技术的实时可控、可逆二氧化硅荧光亚微米线研究
在第一章的基础上,以磷酸化修饰的二氧化硅荧光纳米颗粒为研究对象,通过改变频率、电极间距等因素对其在交流电场下的介电泳行为进行了系统的考察。发现该纳米颗粒可以在间距为20pm的电极间组装成荧光亚微米线。通过控制电场频率,可以很好地控制组装的亚微米线的数目,并且这种亚微米线结构的组装是可逆的。此外,通过将磷酸化修饰的二氧化硅纳米颗粒分散在不同的介质中,发现其介电泳行为对分散介质中的氢离子敏感。该部分研究内容展示了功能化二氧化硅纳米颗粒的介电泳行为的潜在应用前景。
3、不同功能化基团修饰的二氧化硅纳米颗粒对细胞介电性质的影响研究
本章中,以间距不同的叉指式电极阵列作为对细胞介电性质变化的辨别工具,考察了不同功能化二氧化硅纳米颗粒与HeLa细胞共孵育后对细胞介电性质的影响。发现功能化二氧化硅纳米颗粒被HeLa细胞吞噬后可以在细胞内对细胞的介电泳行为和介电性质产生影响。该研究首次探讨了纳米颗粒对细胞介电性质的影响,为研究细胞的微小介电性质的变化提供了方法。
Precise fabrication of controllable and reversible nanostructures or microstructures-based functional devices and systems are of great interest for expanding the potential nanotechnology applications in the areas such as biosensing. Dielectrophoresis (DEP), the movement of polarizable particle induced by a nonhomogeneous AC electric field, has been proven as a robust method to rapidly manipulate and assemble biological and synthetic nanomaterials into nanodevices and mocrosystems. However, due to inadequate understanding of DEP mechanisms, it remains very limited to precisely control the final structure of assembled nanoparticles under DEP. This thesis is aimed at DEP assembly of functionalized silica nanoparticles and its effects on dielectric properties of cells. Precisely controllable and reversible DEP assembled submicrostruct have been achieved by modification of anionic groups on silica nanoparticles, and the effects of intracellular functionalized silica nanoparticles on dielectric properties of cells have been proven. This thesis is composed of the following three parts:
1. Research on effects of different surface functionalized groups on DEP assembly behavior of silica nanoparticles.
The DEP assembly behavior of five types of silica nanoparticles (SiNPs), including OH-SiNPs, COOH-SiNPs, NH2-SiNPs, CH3HPO2-SiNPs and PEG-SiNPs have been investigated respectively. It was found that anionic groups could obviously enhance the DEP assembly behavior of SiNPs on the microelectrodes. The anionic group could bring an increase on the dielectric conductivity of the SiNPs by enhancing the surface conductivity. These results well indicated that the DEP assembly behavior of nanomaterials in aqueous suspensions could been changed by functionalized group modification.
2. Research on controllable and reversible submicrowires assembled from CH3HPO2-SiNPs.
On basis of the work in the first part, the DEP assembly behavior of CH3HPO2-SiNPs was further investigated. By using Rubpy dye doped in the core of the CH3HPO2-SiNPs, the assembly process was visualized real time by inverse fluorescence microscopy. Precise control over the frequency of the applied AC field showed that DEP forces can assemble CH3HPO2-SiNPs from aqueous suspensions into submicrowires and the number of the assembled submicrowires between microelectrode gaps could be well controlled with reversibility. Furthermore, the DEP assembly process of CH3HPO2-SiNPs is sensitive to pH of the dispersed medium. These findings provide a way to solve the difficulty in controlling the DEP assembly process of nanoparticles and offer application opportunities for DEP assembly of functionalized SiNPs.
3. Research on the effects of different functionalized silica nanoparticles on dielectric properties of cells
Electrode arrays with different gap distances were designed to assemble cells with different dielectric properties into different region of the electrode arrays. The assembly behavior of Hela cells on the electrode arrays were investigated after incubated with different functionalized silica nanoparticles. It was found the intracellular functionalized silica nanoparticles could obviously change the assembled region of HeLa cells on the electrode arrays, which means the dielectric properties of the cells had been changed. This part of work provides a new method for investigating small dielectric property changes of cells.
1、不同功能基团修饰对二氧化硅纳米颗粒介电泳自组装行为的影响研究
通过对二氧化硅纳米颗粒、羧基化二氧化硅纳米颗粒、磷酸化二氧化硅纳米颗粒、PEG化二氧化硅纳米颗粒和氨基化二氧化硅纳米颗粒在交流电场下的介电泳自组装行为进行考察,发现带较强负电荷的功能化基团修饰可以有效地增强二氧化硅纳米颗粒在微电极上的自组装行为。其原因是带较强负电荷的功能化基团能增强二氧化硅纳米颗粒表面的阳离子扩散层,从而提高其表面电导率。这为有针对性地改善纳米颗粒在水溶液中的介电性质,使其更好进行介电泳白组装提供了有力的实验依据。
2、基于介电泳技术的实时可控、可逆二氧化硅荧光亚微米线研究
在第一章的基础上,以磷酸化修饰的二氧化硅荧光纳米颗粒为研究对象,通过改变频率、电极间距等因素对其在交流电场下的介电泳行为进行了系统的考察。发现该纳米颗粒可以在间距为20pm的电极间组装成荧光亚微米线。通过控制电场频率,可以很好地控制组装的亚微米线的数目,并且这种亚微米线结构的组装是可逆的。此外,通过将磷酸化修饰的二氧化硅纳米颗粒分散在不同的介质中,发现其介电泳行为对分散介质中的氢离子敏感。该部分研究内容展示了功能化二氧化硅纳米颗粒的介电泳行为的潜在应用前景。
3、不同功能化基团修饰的二氧化硅纳米颗粒对细胞介电性质的影响研究
本章中,以间距不同的叉指式电极阵列作为对细胞介电性质变化的辨别工具,考察了不同功能化二氧化硅纳米颗粒与HeLa细胞共孵育后对细胞介电性质的影响。发现功能化二氧化硅纳米颗粒被HeLa细胞吞噬后可以在细胞内对细胞的介电泳行为和介电性质产生影响。该研究首次探讨了纳米颗粒对细胞介电性质的影响,为研究细胞的微小介电性质的变化提供了方法。
Precise fabrication of controllable and reversible nanostructures or microstructures-based functional devices and systems are of great interest for expanding the potential nanotechnology applications in the areas such as biosensing. Dielectrophoresis (DEP), the movement of polarizable particle induced by a nonhomogeneous AC electric field, has been proven as a robust method to rapidly manipulate and assemble biological and synthetic nanomaterials into nanodevices and mocrosystems. However, due to inadequate understanding of DEP mechanisms, it remains very limited to precisely control the final structure of assembled nanoparticles under DEP. This thesis is aimed at DEP assembly of functionalized silica nanoparticles and its effects on dielectric properties of cells. Precisely controllable and reversible DEP assembled submicrostruct have been achieved by modification of anionic groups on silica nanoparticles, and the effects of intracellular functionalized silica nanoparticles on dielectric properties of cells have been proven. This thesis is composed of the following three parts:
1. Research on effects of different surface functionalized groups on DEP assembly behavior of silica nanoparticles.
The DEP assembly behavior of five types of silica nanoparticles (SiNPs), including OH-SiNPs, COOH-SiNPs, NH2-SiNPs, CH3HPO2-SiNPs and PEG-SiNPs have been investigated respectively. It was found that anionic groups could obviously enhance the DEP assembly behavior of SiNPs on the microelectrodes. The anionic group could bring an increase on the dielectric conductivity of the SiNPs by enhancing the surface conductivity. These results well indicated that the DEP assembly behavior of nanomaterials in aqueous suspensions could been changed by functionalized group modification.
2. Research on controllable and reversible submicrowires assembled from CH3HPO2-SiNPs.
On basis of the work in the first part, the DEP assembly behavior of CH3HPO2-SiNPs was further investigated. By using Rubpy dye doped in the core of the CH3HPO2-SiNPs, the assembly process was visualized real time by inverse fluorescence microscopy. Precise control over the frequency of the applied AC field showed that DEP forces can assemble CH3HPO2-SiNPs from aqueous suspensions into submicrowires and the number of the assembled submicrowires between microelectrode gaps could be well controlled with reversibility. Furthermore, the DEP assembly process of CH3HPO2-SiNPs is sensitive to pH of the dispersed medium. These findings provide a way to solve the difficulty in controlling the DEP assembly process of nanoparticles and offer application opportunities for DEP assembly of functionalized SiNPs.
3. Research on the effects of different functionalized silica nanoparticles on dielectric properties of cells
Electrode arrays with different gap distances were designed to assemble cells with different dielectric properties into different region of the electrode arrays. The assembly behavior of Hela cells on the electrode arrays were investigated after incubated with different functionalized silica nanoparticles. It was found the intracellular functionalized silica nanoparticles could obviously change the assembled region of HeLa cells on the electrode arrays, which means the dielectric properties of the cells had been changed. This part of work provides a new method for investigating small dielectric property changes of cells.
引文
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