Ultra-smooth and crystalline uniform gold nanospheres with biocompatible ability
저자
발행사항
Seoul : Sungkyunkwan university, 2019
학위논문사항
Thesis (Ph.D.)-- Sungkyunkwan university : Department of Chemical Engineering 2019. 8
발행연도
2019
작성언어
영어
주제어
발행국(도시)
서울
기타서명
생체에 적합성을 갖는 완전 구형 금 나노입자
형태사항
xv, 161 p. : ill., charts ; 30 cm
일반주기명
Adviser: Gi-Ra Yi
Includes bibliographical reference(p. 139-158)
UCI식별코드
I804:11040-000000155732
DOI식별코드
소장기관
Gold nanoparticles (GNPs) have been widely employed in optical and biological applications due to their unique optical properties, easiness of surface functionalization, chemical stability, and low toxicity. Spherical GNPs show size-dependent localized surface Plasmon resonance, which leads to unique photothermal effect due to non-radiative relaxation. Due to thiol-gold chemistry, various biological molecules such as oligonucleotides, antibodies, proteins, and DNA were functionalized on their surface, which provides a platform for the recognition of specific target chemical or biomolecules or their programmed self-assembly. However, conventional synthetic methods produced in general faceted or polydisperse gold nanoparticles or complicated and slow synthetic process may produce uniform spherical particles with extremely low yield. To address this problem, novel synthetic route to ultra-smooth and crystalline gold nanosphere (GNS) was developed, in which octahedron nanoparticles were chemically etched forming nanospheres at the presence of positive polyelectrolytes on their surface. In this dissertation, we present the large-scale synthesis of gold nanospheres and then surface modification for further biological applications.
In Chapter 2, the large-scale synthesis of GNSs was described of which reaction volume was larger than previous report by 20 times. More importantly, several experimental factors for controlling size of uniform GNS ranging from 38 to 110 nm were investigated which include pressure, the concentrations of polyDADMAC, and reaction temperature. In Chapter 3, those GNS were modified with PEG by repeated washing and redispersion with thiolated PEG solution and their photothermal effect were investigated depending on its morphology and size distribution through the comparing PEG-coated gold nanospheres (S-GNSs) and commercially available ordinary gold nanoparticles (O-GNPs). Since the light absorption of GNSs is one of the key parameters in photothermal effect, which is dependent of the morphology of gold nanoparticles, their three-dimensional morphologies were carefully analyzed by electron tomography technique and their absorption cross-section was computed from Mie theory considering morphological and distributional factors. We found that uniform gold nanospheres show much higher efficiency than ordinary gold nanoparticles as predicted in simulation results. In Chapter 4, GNSs were investigated as the cell cycle regulator after the surface modification with NH2-PEG (N-GNS). N-GNSs are rapidly introduced on the bottom of fibronectin-coated cell-growth dish due to charge interaction between the amine group and fibronectin, which would work as nanobarrier of cell growth. Three different GNSs with the diameter of 42, 83, and 111 nm were tested as nanobarrier to investigate the size-dependent effect in cell cycle as well as cell cytotoxicity. Among them, only 83-nm GNSs could regulate cell cycle including mitosis due to nanobarrier without toxicity. Finally, in Chapter 5, the surface modification process of GNSs was further developed for the introduction of DNA on PEG brushes. DNA cannot be directly introduced on the positively charged surface of GNSs due to an opposite charge. Therefore, in order to keep the colloidal stability during surface modification, GNSs were first modified by SH-PEG-NH2 with the removal of polyDADMAC and then amine groups on PEG chains were coupled with sulfo-SMCC leaving maleimide groups of sulfo-SMCC which were finally conjugated with thiolate DNA by thiol-ene click chemistry. DNA-coated gold nanospheres were selectively coated on nanopatterned glass substrates with complementary DNA.
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