本文選題：三維氮雜石墨烯 + 納米復(fù)合材料��； 參考：《江蘇大學(xué)》2017年碩士論文

【摘要】：三維氮雜石墨烯(3DNG)不僅具有NG良好的物理化學(xué)性能,而且具有孔隙豐富、導(dǎo)電性好和比表面積大等獨特優(yōu)勢,因此被視為一種很好的支撐載體。3DNG基復(fù)合材料優(yōu)異的電化學(xué)性能已在電化學(xué)領(lǐng)域引起關(guān)注。本論文以三維氮雜石墨烯水凝膠(3DNGH)為載體,通過水熱法制備了多種復(fù)合材料,并考察了其在電催化甲醇氧化、光電化學(xué)(PEC)傳感和電化學(xué)發(fā)光(ECL)生物傳感等領(lǐng)域的應(yīng)用,取得了一些有益的結(jié)果,主要內(nèi)容如下:1、采用簡單的一步水熱法制備了Pt納米粒子負(fù)載的3DNGH(PtNPs/3DNGH)。由多種表征手段可知,所得納米復(fù)合物呈明顯的3D多孔結(jié)構(gòu),PtNPs粒徑大約為2-3 nm,且尺寸均一,分散性好。電化學(xué)性能研究表明,PtNPs/3DNGH與PtNPs/3D石墨烯和PtNPs/石墨烯相比,電化學(xué)活性面積分別為42.17 m2/g、19.18 m2/g和12.05m2/g。PtNPs/3DNGH電催化甲醇氧化的效率依次是其余二者的1.6倍和2.2倍。因此,該催化劑具有較好的催化性能,在未來高性能燃料電池中具有潛在的應(yīng)用價值。2、采用簡單的一步水熱法制備了ZnO/3DNGH。與制備的ZnO/3D石墨烯和ZnO/NG的PEC性能對比研究發(fā)現(xiàn),ZnO/3DNGH光電流強度是前者的1.5倍和2.1倍。這是由于3DNGH具有更大的比表面積,可以負(fù)載更多的Zn O納米顆粒,同時氮的摻入提高了其導(dǎo)電性能,從而提高了其光電流強度。因為該材料具有比表面大、導(dǎo)電性好等優(yōu)異性能,且可負(fù)載更多的生物識別分子。進(jìn)一步以ZnO/3DNGH為載體,以辣根過氧化物酶(HRP)為模型酶,基于HRP在H_2O_2存在下,可以催化氧化4-氯-1-萘酚產(chǎn)生沉淀覆蓋于ZnO/3DNGH的表面,導(dǎo)致PEC信號抑制的作用原理,構(gòu)建了H_2O_2傳感器。該傳感器的光電流強度與H_2O_2濃度在0.001~5 mM范圍內(nèi)呈現(xiàn)良好的線性關(guān)系,檢出限為3μM(S/N=3)。基于此平臺,進(jìn)一步構(gòu)建了雙酶PEC生物傳感應(yīng)用于b-D(+)-葡萄糖的檢測,其檢出限低至0.66μM(S/N=3)。該傳感器具有穩(wěn)定性高和重現(xiàn)性好等特點,可用于葡萄糖的靈敏快速地檢測。3、通過簡單的水熱法制備了AgBr/3DNGH。研究結(jié)果表明,與AgBr負(fù)載的三維石墨烯水凝膠、3DNGH和AgBr/NG相比,AgBr/3DNGH作為魯米諾(luminol)固定載體的ECL強度是前者的2、3和8倍。這是由于3D多孔結(jié)構(gòu)可以提供較大的比表面積負(fù)載luminol分子,氮的摻入可以改善其導(dǎo)電性,AgBr對luminol的ECL起到催化作用等影響,從而提高了其ECL強度。進(jìn)一步以制備的luminol/AgBr/3DNGH作為載體,以戊二醛為交聯(lián)劑固定適配體,基于適配體與大腸桿菌(E.coli)之間能發(fā)生特異性結(jié)合進(jìn)而使其ECL強度受到抑制的機(jī)理,構(gòu)建了超靈敏的E.coli適配體傳感器。該傳感器對E.coli的響應(yīng)范圍在0.5~500 cfu/mL,檢出限為0.17 cfu/mL(S/N=3),并成功地應(yīng)用于牛奶樣品的檢測。
[Abstract]:3DNGs not only have good physical and chemical properties, but also have unique advantages such as rich porosity, good electrical conductivity and large specific surface area. Therefore, the excellent electrochemical properties of 3DNG matrix composites, which are regarded as a good support carrier, have attracted much attention in the field of electrochemistry. In this paper, a variety of composite materials were prepared by hydrothermal method, and their applications in the fields of electrocatalytic methanol oxidation, photochemical PECs sensing and electrochemiluminescence (ECL) biosensor were investigated. Some useful results have been obtained. The main contents are as follows: 1. The Pt nanoparticles supported 3DNGHN PtNPs / 3DNGH have been prepared by a simple one-step hydrothermal method. The results show that the PtNPs with 3D porous structure are about 2-3 nm in size, uniform in size and good in dispersion. The electrochemical performance of PtNPs / 3DNGH was compared with that of PtNPs/3D graphene and PtNPs/ graphene. The electrochemical activity area of PtNPs / 3DNGH was 42.17 m2 / g 19.18 m2 / g and the efficiency of 12.05m2/g.PtNPs/3DNGH electrocatalytic methanol oxidation was 1.6 and 2.2 times of that of the other two, respectively. Therefore, the catalyst has good catalytic performance, and has potential application value in high performance fuel cells in the future. ZnO / 3DNGH was prepared by a simple one-step hydrothermal method. Compared with the PEC properties of ZnO/3D graphene and ZnO/NG, it is found that the photocurrent intensity of ZnO / 3DNGH is 1.5 and 2.1 times higher than that of the former. This is due to the fact that 3DNGH has a larger specific surface area and can support more Zn-O nanoparticles, while nitrogen incorporation improves its electrical conductivity, thus increasing its photocurrent intensity. Because the material has large surface, good conductivity and other excellent properties, and can support more biometric molecules. Furthermore, using ZnO/3DNGH as carrier and horseradish peroxidase (HRP) as model enzyme, a H_2O_2 sensor was constructed based on the mechanism that 4-chloro-1-naphthol could be oxidized on the surface of ZnO/3DNGH by catalyzing the oxidation of 4-chlor-1-naphthol in the presence of H_2O_2, which led to the inhibition of PEC signal. The optical current intensity of the sensor has a good linear relationship with the concentration of H_2O_2 in the range of 0.001 ~ 5 mm, and the detection limit is 3 渭 m ~ (-1) S / N ~ (3 +). Based on this platform, a double enzyme PEC biosensor was further constructed for the detection of b-D (N-glucose). The detection limit of the biosensor was as low as 0.66 渭 m ~ (-1) S / N ~ (3 +). The sensor has the advantages of high stability and good reproducibility. It can be used for the sensitive and rapid detection of glucose. AgBr-3DNGH was prepared by a simple hydrothermal method. The results show that the ECL intensity of Ag-Br-3-DNGH as a luminol fixed carrier is 2 ~ 3 and 8 times higher than that of AgBr supported three-dimensional graphene hydrogel (3DNGH) and AgBr/NG. This is due to the fact that 3D porous structure can provide a large specific surface area to support the luminol molecule, and the incorporation of nitrogen can improve its electrical conductivity, such as its catalytic effect on the ECL of luminol, thus increasing its ECL strength. Furthermore, luminol/AgBr/3DNGH was used as carrier and glutaraldehyde as crosslinking agent to immobilize aptamer. Based on the mechanism of specific binding between aptamer and E. coli, the strength of ECL was inhibited. A super sensitive E.coli aptamer sensor was constructed. The response range of the sensor to E.coli is 0.5 ~ 500cfu-mL, and the detection limit is 0.17 cfu-mL ~ (-1) S / N ~ (3 +), which has been successfully applied to the detection of milk samples.
【學(xué)位授予單位】：江蘇大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TB383.1;O657.1

【參考文獻(xiàn)】

相關(guān)期刊論文 前1條

1 ;Progress in the studies of photoelectrochemical sensors[J];Science in China(Series B:Chemistry);2009年11期

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本文編號：1957794