【摘要】：氧化石墨烯基銀納米顆粒(Ag NPs/GO)復合材料具有優(yōu)異的物化性質(zhì),從而在光學、醫(yī)藥、催化等領(lǐng)域具有廣闊的應(yīng)用前景。但目前Ag NPs/GO復合材料的制備路線中均通過超聲剝離氧化石墨的方法獲得GO,會顯著減小GO的片層尺寸,同時過量加入的表面活性劑或功能化試劑會造成Ag NPs的結(jié)構(gòu)缺陷,從而不利于材料整體性能的發(fā)揮。此外,在現(xiàn)有的制備路線中還存在過程復雜、污染嚴重、能耗大等問題,不利于材料的可控宏觀制備。因此,Ag NPs/GO復合材料的制備仍然面臨著巨大的挑戰(zhàn)。60Co伽馬(γ)射線輻照技術(shù)不僅具有均勻、高效、低污染的特點,還能夠在較高的輻照劑量下碎化顆粒的尺寸。此外,根據(jù)我們之前的研究表明,γ射線還能誘導層間小分子的生長進而剝離氧化石墨。因此,γ射線輻照法有望成為Ag NPs/GO復合材料的理想制備方案。本論文結(jié)合γ射線與陽離子交換技術(shù)的優(yōu)勢,通過γ射線輻照層插硝酸咪唑銀的氧化石墨前驅(qū)體,誘導層間Ag NPs的生長,從而同步實現(xiàn)氧化石墨的剝離和Ag NPs的還原生長,高效獲得Ag NPs/GO復合材料。測試結(jié)果表明,通過該路線得到的Ag NPs/GO復合材料具有較高的純度和結(jié)晶規(guī)整度,高負載量的球形Ag NPs單分散在大尺寸GO表面。同時在對照實驗中發(fā)現(xiàn)層間Ag NPs的生長會受到氧化石墨的限制。隨后我們從Ag NPs在GO片層上呈現(xiàn)拋物線分布及Ag NPs的尺寸隨GO層間距的增大而增大兩方面來證實了這種現(xiàn)象(層間限制效應(yīng))。最后我們從Ag NPs晶體的成核與晶核的生長兩個階段來對Ag NPs結(jié)構(gòu)演化進行機理描述,同時認為氧化石墨的層間限制效應(yīng)主要影響Ag NPs的核生長階段,完善了 γ輻照下Ag NPs/GO復合材料的晶體結(jié)構(gòu)演化規(guī)律。為Ag NPs/GO復合材料的宏觀制備提供一個全新的開發(fā)路線和理論基礎(chǔ)。此外,在合適的銀離子濃度下,能夠獲得較大顆粒尺寸(13.93nm)和基底完全剝離的Ag NPs/GO復合材料,在Raman化學增強和電磁增強效應(yīng)的協(xié)同作用下使該材料展現(xiàn)出優(yōu)異的SERS活性,其Raman信號是純GO的6.3倍。該Ag NPs/GO復合材料制備成的基底對CV的檢測靈敏度為10-7、EF=1.3 × 106,表明該SERS基底能夠應(yīng)用于有機染料的檢測。
[Abstract]:Because of its excellent physicochemical properties, graphene oxide silver nanoparticles (Ag NPs/GO) composites have wide applications in optics, medicine, catalysis and so on. However, at present, in the preparation of Ag NPs/GO composites, GO, can be obtained by ultrasonic stripping of graphite oxide, and the lamellar size of GO will be significantly reduced. At the same time, excessive addition of surfactants or functionalization reagents will lead to the structure defects of Ag NPs. This is not conducive to the performance of the overall properties of the material. In addition, there are some problems in the existing preparation route, such as complex process, serious pollution and high energy consumption, which is not conducive to the controllable macroscopic preparation of materials. Therefore, the preparation of Ag NPs/GO composites is still facing a great challenge. 60Co gamma (緯) irradiation technology not only has the characteristics of uniform, high efficiency and low pollution, but also can be used to break the size of particles at high irradiation dose. In addition, according to our previous studies, 緯 -rays can also induce the growth of interlaminar small molecules and peel off graphite oxide. Therefore, 緯-ray irradiation is expected to be an ideal preparation method for Ag NPs/GO composites. Combining the advantage of 緯 -ray and cationic exchange technology, this paper induces the growth of interlaminar Ag NPs through 緯 -ray irradiation layer intercalation of silver nitrate with imidazole silver oxide, thus realizing the simultaneous exfoliation of graphite oxide and the reduction growth of Ag NPs. Ag NPs/GO composites were obtained efficiently. The test results show that the Ag NPs/GO composites obtained by this route have high purity and crystallinity, and spherical Ag NPs with high loading amount are monodisperse on the surface of large size GO. At the same time, it was found that the growth of interlaminar Ag NPs was limited by graphite oxide. Then we confirm this phenomenon from two aspects: the parabola distribution of Ag NPs on the GO layer and the increase of the size of Ag NPs with the increase of GO spacing. Finally, we describe the mechanism of Ag NPs structure evolution from two stages of nucleation and nucleation of Ag NPs crystal. At the same time, we think that the interlaminar confinement effect of graphite oxide mainly affects the nuclear growth stage of Ag NPs. The evolution law of crystal structure of Ag NPs/GO composites under 緯 -irradiation was improved. It provides a new development route and theoretical basis for macroscopical preparation of Ag NPs/GO composites. In addition, large particle size (13.93nm) and completely stripped Ag NPs/GO composites can be obtained under the appropriate silver ion concentration. Under the synergistic effect of chemical and electromagnetic enhancement of Raman, the material exhibited excellent SERS activity, and its Raman signal was 6.3 times that of pure GO. The sensitivity of the substrate prepared by the Ag NPs/GO composite to the detection of CV is 10 ~ (-7) F _ (1. 3) 脳 10 ~ (6), which indicates that the SERS substrate can be applied to the detection of organic dyes.
【學位授予單位】：天津工業(yè)大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TB33

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