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光輻照制備各向同性和各向異性銀納米顆粒及機(jī)理分析

發(fā)布時(shí)間:2019-03-20 08:39
【摘要】:以金、銀為代表的貴金屬納米顆粒是現(xiàn)代材料科學(xué)、微納光學(xué)、生物光子學(xué)等前沿科技領(lǐng)域的研究熱點(diǎn),制備具有不同形貌的貴金屬納米顆粒則是實(shí)現(xiàn)納米顆粒性能調(diào)控的一個(gè)重要方法。而相對(duì)于較穩(wěn)定的金納米材料而言,銀納米材料表面形貌控制一直是此領(lǐng)域的難點(diǎn)。在傳統(tǒng)化學(xué)制備方法中,一方面,難以通過(guò)控制晶面生長(zhǎng)得到規(guī)則球形的銀納米顆粒,另一方面,制備具有良好性能的各向異性銀納米材料條件復(fù)雜且苛刻。本文就光輻照法制備各向同性和各向異性銀納米顆粒進(jìn)行研究,發(fā)展出新型光輻照制備與表征方法,探討并分析了產(chǎn)物形成機(jī)制及其表面等離子體特性。首先,利用簡(jiǎn)單的檸檬酸鈉還原法制備了形貌不規(guī)則、尺寸分布于80-90 nm的銀納米顆粒,隨后使用248 nm準(zhǔn)分子激光輻照該納米顆粒溶膠,制備得到規(guī)則球形各向同性顆粒。在使用TEM、SEM、吸收光譜等方式對(duì)產(chǎn)物進(jìn)行表征之后,得到了可靠的制備條件。在形貌的表征中,提出“圓度”來(lái)定量描述納米顆粒接近于規(guī)則球形程度。在機(jī)理的分析中,采用了改進(jìn)的“光熱-相變”理論對(duì)實(shí)驗(yàn)的物理過(guò)程進(jìn)行了詳細(xì)闡述。作為對(duì)比,采用汞燈和氙燈兩種連續(xù)光源分別對(duì)不規(guī)則形貌銀納米顆粒進(jìn)行紫外和可見(jiàn)光波段輻照。在不同的實(shí)驗(yàn)條件下制備出棒狀、三角板狀等各向異性銀納米顆粒。在對(duì)產(chǎn)物進(jìn)行性能表征之后,得到了不同形貌納米顆粒的制備參數(shù)。對(duì)于納米顆粒由不規(guī)則向各向異性的轉(zhuǎn)變過(guò)程,結(jié)合實(shí)驗(yàn)結(jié)果分析其物理機(jī)制,提出了“碎裂-連接-生長(zhǎng)”的演化模型。此外,分析了脈沖激光和連續(xù)光源對(duì)銀納米顆粒表面形貌改變的異同,并對(duì)以上兩部分工作的中的納米顆粒產(chǎn)物進(jìn)行表面增強(qiáng)拉曼散射(SERS)性能表征。實(shí)驗(yàn)結(jié)果表明,規(guī)則球形和各向異性銀納米顆粒均有優(yōu)異的SERS活性,對(duì)探針?lè)肿拥牟煌鶊F(tuán)有選擇性吸附和增強(qiáng)效應(yīng),在痕量物質(zhì)檢測(cè)領(lǐng)域具有廣闊的應(yīng)用前景。
[Abstract]:Precious metal nanoparticles, represented by gold and silver, are the focus of research in modern material science, micro / nano optics, biophotonics and other cutting-edge science and technology fields. The preparation of precious metal nanoparticles with different morphologies is an important method to control the properties of nano-particles. Compared with the stable gold nanomaterials, the surface morphology control of silver nanomaterials has always been a difficulty in this field. In traditional chemical preparation methods, on the one hand, it is difficult to obtain regular spherical silver nanoparticles by controlling the growth of crystal faces. On the other hand, the conditions for preparing anisotropic silver nanoparticles with good properties are complex and demanding. In this paper, the preparation of isotropic and anisotropic silver nanoparticles by light irradiation has been studied. A new method of preparation and characterization of silver nanoparticles by light irradiation has been developed. The formation mechanism and surface plasma characteristics of the products have been discussed and analyzed. Firstly, silver nanoparticles with irregular morphology and size distribution of 80 ~ 90 nm were prepared by a simple sodium citrate reduction method. Then regular spherical isotropic particles were prepared by irradiation of the nanoparticles with 248nm excimer laser. After the product was characterized by TEM,SEM, absorption spectrum and other methods, reliable preparation conditions were obtained. In the characterization of morphology, "roundness" is proposed to quantitatively describe the degree of sphericity of nanoparticles close to that of regular sphericity. In the analysis of the mechanism, the physical process of the experiment is described in detail by using the improved "photothermal-phase transition" theory. As a contrast, mercury lamp and xenon lamp were used to irradiate irregularly shaped silver nanoparticles in ultraviolet and visible wavelengths, respectively. Anisotropic silver nanoparticles, such as rod and triangular plate, were prepared under different experimental conditions. After characterization of the products, the preparation parameters of the nanoparticles with different morphologies were obtained. For the transition process from irregular to anisotropic, the physical mechanism of nano-particles is analyzed, and the evolution model of "fragmentation-connection-growth" is put forward. In addition, the similarities and differences between pulsed laser and continuous light source on the surface morphology of silver nanoparticles were analyzed, and the surface enhanced Raman scattering (SERS) properties of the nanoparticles produced in the above two parts of work were characterized by surface enhanced Raman scattering (SERS). The experimental results show that both regular spherical and anisotropic silver nanoparticles have excellent SERS activity, and have selective adsorption and enhancement effects on different groups of probe molecules. Therefore, they have broad application prospects in the field of trace substances detection.
【學(xué)位授予單位】:北京工業(yè)大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2016
【分類號(hào)】:O614.122;TB383.1

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