【摘要】：電化學(xué)傳感器是指在電極和電解液異相相接的界面上,因電荷的遷移而發(fā)生的電極反應(yīng),從而將響應(yīng)信號(hào)轉(zhuǎn)化為電信號(hào)的化學(xué)傳感器。電化學(xué)傳感器在分析檢測(cè)領(lǐng)域逐漸成為重要的檢測(cè)技術(shù),因其具操作簡(jiǎn)便、選擇性高、分析速度快、價(jià)格低廉、并且可進(jìn)行在線分析等傳統(tǒng)分析方法不可比擬的優(yōu)勢(shì),已經(jīng)在藥理學(xué)、環(huán)境、食品、醫(yī)藥研發(fā)、農(nóng)業(yè)、發(fā)酵工業(yè)生產(chǎn)等領(lǐng)域得到了高度的關(guān)注和廣泛的應(yīng)用。自2010年,Andre Geim和Konstantin Novoselov獲得諾貝爾物理學(xué)獎(jiǎng),國內(nèi)外對(duì)石墨烯倍受關(guān)注。本論文制備了石墨烯及功能化石墨烯雜化材料,并探究了其在電化學(xué)傳感器制備中的應(yīng)用。主要研究了石墨烯及其功能化復(fù)合物作為電極材料在毛細(xì)管電化學(xué)發(fā)光、葡萄糖生物傳感器和P450酶生物傳感器制備中的應(yīng)用,實(shí)現(xiàn)了對(duì)5-羥色胺和酪胺酸、葡萄糖、以及非那西丁的測(cè)定。全文共分為四章:第一章:簡(jiǎn)要介紹了電化學(xué)傳感器的實(shí)際應(yīng)用,綜述了在電化學(xué)傳感器以石墨烯修飾電極的研究進(jìn)展。第二章:通過將三(2,2'-聯(lián)吡啶)釕(Ru(bpy)32+)結(jié)合2,2-連氮基-雙(3-乙基苯并噻唑-6-磺酸)(ABTS)功能化的石墨烯,并且成功的固定在電極表面,制備了一種具有高穩(wěn)定性電致發(fā)光電極。Ru(bpy)32+與ABTS功能化的石墨電極之間的結(jié)合除了π-π電子的共軛作用外,還有靜電作用力。連有毛細(xì)管電泳的電化學(xué)發(fā)光(ECL)傳感器被用于檢測(cè)酪氨酸和5-羥色胺,利用它們對(duì)Ru(bpy)32+/三丙胺(TPA)體系產(chǎn)生淬滅效應(yīng)的。在經(jīng)過對(duì)毛細(xì)管電泳分離和ECL檢測(cè)條件進(jìn)行優(yōu)化后,這種淬滅機(jī)制得到了證實(shí)。在信噪比為S/N=3時(shí),針對(duì)酪氨酸和5-羥色胺的檢測(cè)線分別為0.1μM和0.02μM。此種方法將來可被用于檢測(cè)小腸癌患者中血液內(nèi)的酪氨酸和5-羥色胺。第三章:通過制備聚二烯二甲基氯化銨(PDDA)功能化石墨烯(G),使其表面帶正電,與帶負(fù)電的納米金(Au NPs),進(jìn)行靜電自組裝,制得Au NPs/G。為了驗(yàn)證這種材料的應(yīng)用性,將其修飾到玻碳電極上,以葡萄糖氧化酶(GOD)作為模板。將制備的G/Au NPs/GOD/GCE作為葡萄糖傳感器,其平均電子轉(zhuǎn)移速率為1.64 s-1。制備的葡萄糖傳感器對(duì)葡萄糖的響應(yīng)范圍是1~9m M,檢出限為0.1m M(S/N=3)。這種傳感器能夠有效的排除一般共存化合物的干擾,并且可以對(duì)血清樣品進(jìn)行測(cè)定,其回收率為在95.7%~107.6%。因此,可以說明G/Au NPs雜化材料為GOD提供了優(yōu)良的導(dǎo)電性和適宜的微環(huán)境,這也為固定其他的酶或蛋白質(zhì)提供一種有利的平臺(tái)。第四章:本章主要是將P450酶固定在修飾電極上。通過制備以陽離子聚丙烯酰胺功能化的石墨烯材料,利用材料的物理化學(xué)性質(zhì)固定P4501A2酶,從而研究對(duì)藥物的代謝。制備的CYP1A2/CPAM-G/GCE的對(duì)非那西丁響應(yīng)的靈敏度為1.333μA(μmol/L)-1cm-2,檢出限5.57μmol/L。同時(shí),構(gòu)建的CYP450酶電化學(xué)傳感不僅具有評(píng)價(jià)藥物相互作用的潛能,而且還能為體外構(gòu)建其他生物分子體系提供參考價(jià)值。
[Abstract]:Electrochemical sensor refers to the electrode reaction due to the transfer of charge on the interface between electrode and electrolyte, so as to convert the response signal into electrical signal. Electrochemical sensor has gradually become an important detection technology in the field of analysis and detection, because it has incomparable advantages over traditional analysis methods, such as simple operation, high selectivity, fast analysis speed, low price, and on-line analysis. It has been highly concerned and widely used in pharmacology, environment, food, pharmaceutical research and development, agriculture, fermentation industry and other fields. Since, Andre Geim and Konstantin Novoselov won the Nobel Prize in Physics in 2010, graphene has attracted much attention at home and abroad. In this paper, graphene and functional fossil graphene hybrid materials were prepared and their applications in the preparation of electrochemical sensors were discussed. The application of graphene and its functional complexes as electrode materials in the preparation of capillary electrochemiluminescence, glucose biosensor and P450 enzyme biosensor was studied. And the determination of phenacetin. The full text is divided into four chapters: in the first chapter, the practical application of electrochemical sensor is briefly introduced, and the research progress of graphene modified electrode in electrochemical sensor is reviewed. In chapter 2, graphene functionalized by tris (2, 2 脳 bipyridine) ruthenium (Ru (bpy) 32), 2-nitro-bis (3-ethylbenzothiazole-6-sulfonic acid) was successfully fixed on the surface of the electrode, A highly stable electroluminous electrode was prepared. The binding of Ru (bpy) 32 to ABTS functionalized graphite electrode has electrostatic force in addition to the conjugated 蟺-蟺 electrons. The electrochemiluminescence (ECL) sensor with capillary electrophoresis was used to detect tyrosine and serotonin, and they were used to quench Ru (bpy) 32 / tripropylamine (TPA) system. After optimizing the separation and ECL detection conditions of capillary electrophoresis, the quenching mechanism was confirmed. When the signal-to-noise ratio (SNR) is S/N=3, the detection lines for tyrosine and serotonin are 0.1 渭 M and 0.02 渭 m, respectively. This method can be used to detect tyrosine and serotonin in the blood of patients with small bowel cancer in the future. In chapter 3, Au NPs/G. was prepared by preparing polydiene dimethyl ammonium chloride (PDDA) functional fossil Moene (G), with positive electricity on its surface and electrostatic self-assembly with negative gold (Au NPs),. In order to verify the application of this material, it was modified to glassy carbon electrode and glucose oxidase (GOD) was used as template. Using the prepared G/Au NPs/GOD/GCE as glucose sensor, the average electron transfer rate is 1.64 s 鈮，

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