發(fā)布時間：2018-06-08 12:34

  本文選題：石墨烯 + 碳納米管��； 參考：《濟(jì)南大學(xué)》2017年碩士論文

【摘要】：本論文以碳材料為基底,將金屬材料修飾在碳材料基底表面,使制備的碳基金屬復(fù)合材料具有碳材料比表面積大,導(dǎo)電性能好,機(jī)械性能強(qiáng)以及金屬材料良好的電子傳遞性能,催化性能好等優(yōu)點(diǎn),將制備的碳基金屬復(fù)合材料應(yīng)用于電化學(xué)傳感分析中,對食品藥品進(jìn)行檢測。本論文的研究內(nèi)容分如下幾部分:(1)采取修正的Hummers方法合成了氧化石墨烯,并將氧化石墨烯通過NaBH4還原成石墨烯。利用靜電作用,將聚二丙烯基二甲基氯化銨(PDDA)作用在石墨烯表面,得到PDDA功能化的薄層石墨烯。而后采用水熱合成法制備具有強(qiáng)吸附性能的Al_2O_3,然后將納米金還原在Al_2O_3表面,得到Al_2O_3-Au金屬復(fù)合材料,最后將Al_2O_3-Au修飾在PDDA功能化石墨烯表面,獲得Al_2O_3-Au/PDDA/rGO復(fù)合材料。采用掃描電鏡、X-射線粉末衍射和傅里葉變換紅外光譜等手段對制備的材料表征。將制備的Al_2O_3-Au/PDDA/rGO復(fù)合功能材料涂抹在玻碳電極上,構(gòu)建基于PDDA功能化石墨烯負(fù)載Al_2O_3-Au的電化學(xué)傳感器。對構(gòu)建的電化學(xué)傳感器的電化學(xué)性質(zhì)進(jìn)行表征,并探究了滴涂量、掃速、pH以及聚集時間等條件對傳感器性能的影響。該傳感器用于乙酰氨基酚的測定線性回歸方程為Ip(μA)=0.3410+0.0359c(μM),R2=0.9970,檢出限為6 nM(S/N=3)�？捎糜诟忻八�、鎮(zhèn)痛藥中對乙酰氨基酚高靈敏、快速檢測。(2)通過縮合和π-π共軛等作用將合成的氧化石墨烯與羧基化的多壁碳納米管復(fù)合在一起,制備三維的碳雜化材料,并用硼氫化鈉作為還原劑處理,獲得石墨烯-多壁碳納米管雜化材料;隨后對其進(jìn)行硅烷化處理,通過Au-S鍵,將制備的納米金包附的二氧化鈦微球負(fù)載在碳雜化材料表面,獲得rGO/MWCNTs/TiO_2-Au復(fù)合材料。采用掃描電鏡、能譜、傅里葉紅外、拉曼光譜以及X-射線衍射等手段對復(fù)合材料表征。并將制備的rGO/MWCNTs/TiO_2-Au復(fù)合材料修飾到玻碳電極表面,構(gòu)建基于雜化碳材料負(fù)載TiO_2-Au的電化學(xué)傳感器。對TiO2-Au/MWCNTs/rGO/GCE傳感器的電化學(xué)性質(zhì)進(jìn)行表征,并探究了TiO_2-Au微球粒徑、TiO_2-Au比重、滴涂量、掃速、pH以及聚集時間等條件對傳感器性能的影響。在最佳實(shí)驗(yàn)條件下繪制工作曲線,得線性方程Ip(μA)=0.0313c(nM)+0.5533,R2=0.9972,檢出限為0.34 nM(S/N=3)�？捎糜谧⑸湟�、尿液等樣品中腎上腺素高靈敏、快速檢測。(3)咪唑類離子液體1-丁基-3-甲基咪唑氫溴鹽與氧化石墨烯通過靜電作用制備1-丁基-3-甲基咪唑功能化的氧化石墨烯,并結(jié)合羧基化的碳納米管,制備分散性良好的GO-IL-CNT復(fù)合材料,并與納米金溶膠混合,通過靜電作用結(jié)合納米金,獲得導(dǎo)電性極好的GO-IL-CNT-AuNPs復(fù)合材料。采取掃描電鏡、傅里葉變換紅外光譜以及X-射線衍射等手段對合成的復(fù)合材料進(jìn)行表征。并將合成的GO-IL-CNT-Au NPs復(fù)合材料滴涂到玻碳電極上,構(gòu)建離子液體功能化的碳材料負(fù)載納米金的電化學(xué)傳感器。利用循環(huán)伏安、交流阻抗等實(shí)驗(yàn)技術(shù)對構(gòu)建的GO-IL-CNT-AuNPs/GCE傳感器的電學(xué)性質(zhì)進(jìn)行表征,并探究了滴涂量,掃速,pH以及聚集時間等條件對GO-IL-CNT-AuNPs/GCE傳感器分析性能的影響。在最佳實(shí)驗(yàn)條件下繪制工作曲線,得線性方程Ip(μA)=1.0678c(nM)+2.5821,R2=0.9990,檢出限為1.5 nM(S/N=3)。可進(jìn)行奶瓶、礦泉水瓶等樣品中殘存的雙酚A高靈敏、快速檢測。(4)用共沉淀和自組裝的技術(shù)一步合成離子液體1-丁基-3-甲基咪唑氫溴鹽功能化的羧基化碳納米管負(fù)載納米銅復(fù)合材料。利用納米銅可與二甲雙胍發(fā)生絡(luò)合作用,將合成的納米復(fù)合材料修飾到玻碳電極表面與電化學(xué)工作站連接構(gòu)建檢測二甲雙胍的MWCNT-IL-CuNPs/GCE傳感器。用掃描電鏡、傅里葉變換紅外光譜以及X-射線衍射等手段對合成的各步復(fù)合材料的表面形態(tài)和功能結(jié)構(gòu)詳細(xì)表征,用電化學(xué)等實(shí)驗(yàn)技術(shù)對各個修飾電極進(jìn)行了電化學(xué)性能研究,并對所構(gòu)建的MWCNT-IL-CuNPs/GCE傳感器進(jìn)行了實(shí)驗(yàn)條件的優(yōu)化。采用循環(huán)伏安和差分脈沖法電化學(xué)技術(shù)探究了二甲雙胍在MWCNT-IL-CuNPs/GCE上的電化學(xué)響應(yīng)。在最佳實(shí)驗(yàn)條件下檢測二甲雙胍,傳感器MWCNT-IL-CuNPs/GCE的線性工作范圍是3 nM-50μM,線性方程Ip(μA)=-1.0620c(μM)-5.4660,R2=0.9991,檢出限為1.0 nM(S/N=3)。復(fù)合材料MWCNT-IL-CuNPs修飾的電極提高了檢測的靈敏度,降低了檢出限、獲得了寬的線性范圍,實(shí)現(xiàn)了對二甲雙胍高效、快速的檢測。
[Abstract]:In this paper, carbon material is used as the substrate to modify the metal material on the surface of the carbon material, so that the carbon based metal composites have the advantages of large carbon material, good electrical conductivity, strong mechanical properties, good electronic transfer properties and good catalytic performance. The carbon based metal composites are applied to the electrochemistry of carbon based metal composites. In the sensing analysis, the food and drug are detected. The research content of this paper is divided into the following parts: (1) the modified Hummers method is adopted to synthesize graphene oxide and the graphite oxide is reduced to graphene through NaBH4. Using electrostatic action, the poly two propylene two methyl ammonium chloride (PDDA) is acted on the surface of graphene, and the function of PDDA is obtained. The thin layer graphene was changed. Then the Al_2O_3 with strong adsorption properties was prepared by hydrothermal synthesis. Then the gold nanoparticles were reduced to the surface of Al_2O_3, and the Al_2O_3-Au metal composite was obtained. Finally, the Al_2O_3-Au was modified on the surface of the PDDA function fossils to obtain the Al_2O_3-Au/PDDA/rGO composite. The scanning electron microscopy and X- ray powder diffraction were used. The properties of the prepared materials were characterized by Fu Liye transform infrared spectroscopy. The prepared Al_2O_3-Au/PDDA/rGO composite functional materials were applied to the glassy carbon electrode to construct an electrochemical sensor based on the Al_2O_3-Au of the PDDA function fossil ink. The electrochemical properties of the constructed electrochemical sensors were characterized, and the coating amount and scanning speed were explored. The effect of pH and aggregation time on the performance of the sensor. The sensor is used for the linear regression equation of acetaminophen determination of Ip (mu A) =0.3410+0.0359c (mu M), R2=0.9970, the detection limit is 6 nM (S/N=3). It can be used in cold drugs and the analgesics are highly sensitive and rapid detection of acetaminophen. (2) the combination of condensation and PI - pi conjugation will be combined. A three dimensional carbon hybrid material was prepared with the carboxylation of the multi walled carbon nanotubes, and the graphene multi wall carbon nanotube hybrid material was obtained by using sodium borohydride as a reductant, and then silanylation was carried out and the nano gold coated titanium dioxide microspheres were loaded in the carbon impurity through the Au-S bond. On the surface of the material, rGO/MWCNTs/TiO_2-Au composite was obtained. The composite was characterized by scanning electron microscope, energy spectrum, Fu Liye infrared, Raman spectroscopy and X- ray diffraction. The prepared rGO/MWCNTs/TiO_2-Au composite was modified to the surface of glass carbon electrode, and the electrochemical sensor based on the hybrid carbon material loaded TiO_2-Au was constructed. The electrochemical properties of the TiO2-Au/MWCNTs/rGO/GCE sensor were characterized, and the effects of the particle size of the TiO_2-Au microspheres, the specific gravity of TiO_2-Au, the coating amount, the sweep speed, the pH and the aggregation time on the performance of the sensor were investigated. The working curves were drawn under the optimum experimental conditions, and the linear equation Ip (A) =0.0313c (nM) +0.5533, R2=0.9972, the detection limit was 0.34 nM ( S/N=3). It can be used for high sensitivity and rapid detection of epinephrine in samples such as injection, urine and other samples. (3) the imidazole ionic liquid 1- butyl -3- methylimidazolium bromide and graphene oxide are prepared by electrostatic action to prepare 1- butyl -3- methylimidazole functionalized graphene oxide, combined with carboxylation of carbon nanotubes, to prepare a good dispersible GO-IL-CNT complex The composite materials are mixed with nanoscale colloid, and the GO-IL-CNT-AuNPs composites with excellent conductivity are obtained by electrostatic interaction and gold nanoparticles. The composite materials are characterized by scanning electron microscopy, Fourier transform infrared spectroscopy and X- ray diffraction. The composite GO-IL-CNT-Au NPs composite is applied to the glassy carbon. At the end, the electrochemical sensor of nano gold loaded with ionic liquid functionalized carbon material was constructed. The electrical properties of the GO-IL-CNT-AuNPs/GCE sensor were characterized by cyclic voltammetry, AC impedance and other experimental techniques, and the analysis performance of the GO-IL-CNT-AuNPs/GCE sensor was investigated by the coating amount, sweep speed, pH and aggregation time. The working curve was drawn under the best experimental conditions. The linear equation Ip (nM) =1.0678c (nM) +2.5821, R2=0.9990, the detection limit was 1.5 nM (S/N=3). The residual bisphenol A in the bottles, mineral water bottles and other samples could be highly sensitive and rapid detection. (4) a one-step synthesis of ionic liquid 1- butyl -3- methidazolium bromide with co precipitation and self-assembly technology. A salt functionalized carboxyl carbon nanotube is loaded with nanoscale copper composite. The nano copper can be used to complexing with metformin. The synthesized nanocomposites are modified to the surface of the glass carbon electrode to connect with the electrochemical workstation to construct the MWCNT-IL-CuNPs/GCE sensor for the detection of metformin. The scanning electron microscope (SEM) and Fourier transform infrared spectroscopy are used. The surface morphology and functional structure of the composite materials are characterized in detail by means of X- ray diffraction. The electrochemical properties of each modified electrode are studied by electrochemical techniques. The experimental conditions are optimized for the MWCNT-IL-CuNPs/GCE sensor constructed by the cyclic voltammetry and differential pulse method. The electrochemical response of metformin on MWCNT-IL-CuNPs/GCE was explored. Under the best experimental conditions, the linear working range of the sensor MWCNT-IL-CuNPs/GCE was 3 nM-50 mu M, the linear equation Ip (mu A) =-1.0620c (mu M) -5.4660, R2=0.9991, the detection limit was 1 nM (S/N=3). The sensitivity of detection is increased, the detection limit is reduced, and a wide linear range is obtained, thus achieving an efficient and rapid detection of metformin.
【學(xué)位授予單位】：濟(jì)南大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TB33;O657.1

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