本文關(guān)鍵詞：基于多功能化納米復(fù)合材料超靈敏檢測尿酸等含氮物質(zhì)的研究　出處：《長沙理工大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 電化學(xué)還原 氧化石墨烯 納米金-殼聚糖聚陽離子 功能化PDDA-鉑納米 多壁碳納米管 碳納米點(diǎn) 電催化氧化

【摘要】：生命活動(dòng)中重要的含氮代謝物如尿酸、神經(jīng)遞質(zhì)如多巴胺和抗氧化劑如抗壞血酸等影響著人類生命活動(dòng)過程中的代謝機(jī)制,尿酸含量異常會(huì)誘發(fā)系列代謝疾病,多巴胺的濃度變化則會(huì)影響人的神經(jīng)系統(tǒng),抗壞血酸則影響人體健康的生理機(jī)制。因此,開發(fā)高靈敏性、高特異性和精確的傳感方法用于生命活動(dòng)中的重要含氮物質(zhì)和抗氧化劑等的定量或定性檢測,對維護(hù)生命活動(dòng)的正常進(jìn)行顯得非常重要。本論文結(jié)合多功能化的納米復(fù)合材料,主要從事尿酸等含氮物質(zhì)檢測方面的研究工作,具體如下:(1)電化學(xué)還原氧化石墨烯/納米金-殼聚糖復(fù)合膜修飾玻碳電極對尿酸的靈敏測定:將氧化石墨烯(GO)在玻碳電極(GCE)表面進(jìn)行直接電化學(xué)還原,再組裝上納米金(AuNP)-殼聚糖(CS)聚陽離子,形成了ERGO/AuNP-CS復(fù)合膜修飾的玻碳電極。采用掃描電子顯微鏡(SEM)表征了不同修飾膜表面的形貌,探討了其對尿酸(UA)分子的DPV行為,發(fā)現(xiàn)ERGO/AuNP-CS復(fù)合膜對UA分子表現(xiàn)出顯著的電催化氧化活性。在0.10 mol/L的緩沖溶液(pH=6.5)中,掃速100mV/s時(shí),該復(fù)合膜修飾電極對UA在濃度為0.0500~110μmol/L范圍具有線性響應(yīng),檢測下限為12.4 nmol/L(S/N=3)。該修飾電極具有良好的選擇性、重現(xiàn)性和穩(wěn)定性,可應(yīng)用于人體血清和尿液樣品中UA的測定,回收率達(dá)到93.8~104.1%。與分光光度法和尿酸酶試劑盒法相比較,測定結(jié)果一致。(2)功能化鉑納米-聚陽離子/電化學(xué)還原的氧化石墨稀復(fù)合膜用于尿酸和抗壞血酸的同時(shí)檢測:制備了聚二烯二甲基氯化銨(PDDA)聚陽離子功能化的鉑納米(Pt NP)材料,將GO在GCE表面進(jìn)行直接電化學(xué)還原,再組裝上PtNP-PDDA復(fù)合膜,形成了功能化PtNP-PDDA/ERGO/GCE復(fù)合膜修飾的玻碳電極。采用透射電子顯微鏡(TEM)表征了不同濃度的聚陽離子功能化的鉑納米粒子,探討了其對尿酸(UA)和抗壞血酸(AA)分子的DPV和CV行為,發(fā)現(xiàn)PtNP-PDDA/ERGO復(fù)合膜對尿酸(UA)和抗壞血酸(AA)分子表現(xiàn)出顯著的電催化氧化活性及電分離作用,尿酸和抗壞血酸無需分離即可同時(shí)被檢測出。在0.10 mol/L的緩沖溶液(pH=5.5)中,掃速為100 mV/s時(shí),其對UA在濃度為0.025~20.0μmol/L范圍具有線性響應(yīng),檢測下限為7.2 nmol/L(S/N=3);對AA的濃度在為2.50~110μmol/L濃度范圍內(nèi)呈線性關(guān)系,檢測下限為0.150μmol/L(S/N=3)。該修飾電極具有良好的抗干擾性、重現(xiàn)性和穩(wěn)定性,可應(yīng)用于人體血清樣品中UA和AA的同時(shí)測定,回收率分別達(dá)到94.2~102.2%和96.9~105.4%。與尿酸酶試劑盒法和熒光光譜分析法相比較,測定結(jié)果令人滿意,說明該修飾電極在生物醫(yī)學(xué)領(lǐng)域有潛在的應(yīng)用價(jià)值。(3)復(fù)合型碳納米點(diǎn)-離子液體復(fù)合納米材料的制備及同時(shí)測定尿酸和亞硝酸鹽:結(jié)合多壁碳納米管(MWCNTs)、離子液體([BMIM]BF4,IL)、氧化石墨烯(GO),采用超聲法制備了一種新穎穩(wěn)定的復(fù)合型氧化石墨烯碳點(diǎn)-碳納米管碳點(diǎn)-離子液體(GQD-CQD-IL)的碳納米點(diǎn)復(fù)合材料。利用透射電鏡(TEM)對所合成的碳納米點(diǎn)材料的形貌進(jìn)行了表征,并研究了UA和NO2-同時(shí)存在于GQD-CQD-IL修飾電極上的CV特性,發(fā)現(xiàn)GQD-CQD-IL修飾電極良好的電催化氧化性能。對尿酸(UA)和亞硝酸鹽(NO2-)分析檢測的線性范圍分別為0.15~20.0μmol/L,0.20~30.0μmol/L,檢測限(S/N=3)分別為0.0062μmol/L,0.036μmol/L。應(yīng)用于實(shí)際樣品中UA和NO_(2-)測定,回收率分別為96.0%~101%,99.8%~102%,與尿酸酶試劑盒法和分光光度法相對比,實(shí)驗(yàn)測試結(jié)果令人滿意,說明該修飾電極在生物分析檢測領(lǐng)域有潛在的應(yīng)用價(jià)值。(4)基于聚陽離子功能化的多壁碳納米管(MWCNTs)高負(fù)載鉑納米粒子(PtNPs)復(fù)合膜對多巴胺的靈敏測定:用PDDA聚陽離子將多壁碳納米管(MWCNTs)的表面進(jìn)行功能化,再通過液相還原法成功地將PtNPs負(fù)載在MWCNTs的表面,構(gòu)建了一種GCE/(MWCNT-PDDA/PtNPs)-Nafion修飾電極。使用TEM表征了不同的復(fù)合材料的形貌,探討了修飾電極對DA的DPV和CV行為,研究發(fā)現(xiàn)MWCNT-PDDA/PtNPs復(fù)合膜對DA分子表現(xiàn)出良好的電催化氧化活性。實(shí)驗(yàn)結(jié)果說明,該修飾電極對多巴胺的電催化的線性范圍為0.01~30μmol/L,檢測限為2.5nmol/L(3S/N)。此外,該電極表現(xiàn)了較強(qiáng)的抗干擾能力、良好的重現(xiàn)性和穩(wěn)定性。這種集碳納米管、聚合電解質(zhì)及貴金屬納米粒子為一體的納米復(fù)合材料的構(gòu)建為多巴胺高效靈敏的電化學(xué)檢測提供了一個(gè)較好的研究平臺(tái)。
[Abstract]:The life activities of important nitrogenous metabolites such as uric acid, neurotransmitters such as dopamine and antioxidants such as ascorbic acid affects the metabolism of human life in the process, the content of uric acid can induce a series of abnormal metabolic diseases, concentration of dopamine will affect the nervous system, affects the physiological mechanism of ascorbic acid in human body. Therefore, the development of high sensitivity, high specificity and accurate sensing method for quantitative or qualitative detection in the life activity of important nitrogenous substances and antioxidant, to maintain the normal activity of life is very important. This paper combines the nanocomposite functional, the main research work, engaged in uric acid nitrogen detection the details are as follows: (1) electrochemical reduction of graphene oxide / gold nanoparticles chitosan composite film glassy carbon electrode for the sensitive determination of uric acid: oxidation Graphene (GO) on a glassy carbon electrode (GCE) surface by direct electrochemical reduction, then assembled on gold nanoparticles (AuNP) - chitosan (CS) polycation, glassy carbon electrode to form ERGO/AuNP-CS composite film modified by scanning electron microscopy (SEM) characterization of the morphology of different surface modification, is discussed the uric acid (UA) DPV molecule, ERGO/AuNP-CS composite membrane of UA molecules exhibited electrocatalytic activity significantly. In the buffer solution of 0.10 mol/L (pH=6.5), scan rate 100mV/s, the composite membrane modified electrode to UA at the concentration of 0.0500~110 mol/L has a range of linear response, detection limit 12.4 nmol/L (S/N=3). The modified electrode has good selectivity, reproducibility and stability, can be applied to the determination of human serum and urine samples in UA, the recovery rate reached 93.8~104.1%. compared with the spectrophotometric method and urine acid enzyme reagent kit method, the determination results . (2) functionalized platinum nano polycation / electrochemical reduction of graphene oxide composite membrane for the detection of uric acid and ascorbic acid at the same time: preparation of polydiene two methyl ammonium chloride (PDDA) cationic poly platinum nano functional materials (Pt NP), GO on the surface of GCE by direct electrochemical reduction. Then the assembly of PtNP-PDDA composite membrane, forming a functionalized glassy carbon electrode PtNP-PDDA/ERGO/GCE composite film modified by transmission electron microscopy (TEM) characterization of platinum nanoparticles functionalized poly cation with different concentrations, to determine the uric acid (UA) and ascorbic acid (AA) molecules DPV and CV, found that PtNP-PDDA/ERGO composite film the uric acid (UA) and ascorbic acid (AA) molecules exhibit significant electrocatalytic activity and electric separation, uric acid and ascorbic acid without separation can also be detected. In the buffer solution of 0.10 mol/L (pH=5.5), Saul The speed is 100 mV/s, the concentration of UA in the 0.025~20.0 mol/L range with a linear response, a detection limit of 7.2 nmol/L (S/N=3); the AA concentration in 2.50~110 mol/L concentration range showed a linear relationship, detection limit of 0.150 mol/L (S/N=3). The modified electrode has good anti interference, reproducibility and stability, can be applied to the determination of UA and AA in human serum samples at the same time, the recovery rate reached 94.2~102.2% and 96.9~105.4%. with uricase Kit Method and fluorescence spectrum analysis method compared with satisfactory results, the modified electric potential application in biomedical field. (3) composite carbon nano - ionic liquid composite nano material preparation and determination of uric acid and nitrite: combination of multi walled carbon nanotubes (MWCNTs), ionic liquid ([BMIM]BF4, IL), graphene oxide (GO), was prepared by a novel ultrasound method The composite type graphene oxide carbon - stable carbon nanotube - ionic liquid (GQD-CQD-IL) carbon nano composites. By using transmission electron microscopy (TEM) morphology of carbon nano materials synthesized were characterized, and the effects of UA and NO2- exist in the GQD-CQD-IL CV characteristics of electrodes. Found that the electrocatalytic oxidation of GQD-CQD-IL modified electrode. The good of uric acid (UA) and nitrite (NO2-). The linear range of analysis were 0.15~20.0 mol/L, 0.20~30.0 mol/L (S/N=3) respectively, the detection limit is 0.0062 mol/L, the application of mol/ L. 0.036 in UA and NO_ in real samples (2-) were measured. The recovery rates were 96.0%~101%, 99.8%~102%, and uricase Kit Method and spectrophotometry were compared, the experimental results is satisfactory, indicating that the modified electrode has potential application value in the field of biological detection and analysis. (4) based on poly cationic The multi walled carbon nanotubes (MWCNTs) high load platinum nanoparticles (PtNPs) composite membrane for the sensitive determination of dopamine by PDDA cationic multi wall carbon nanotubes (MWCNTs) functionalized by surface by liquid phase reduction method PtNPs was successfully loaded on the surface of MWCNTs, constructed a GCE/ (MWCNT-PDDA/PtNPs -Nafion) modified electrode. TEM was used to characterize the different morphologies of the composites, discusses the modified electrode of DA DPV and CV, the study found that MWCNT-PDDA/PtNPs composite membrane of DA molecules exhibit good electrocatalytic activity. The experimental results show that the linear range of the modified electrode electrocatalysis to dopamine for 0.01~30. Mol/L, the detection limit is 2.5nmol/L (3S/N). In addition, the electrode has a strong anti-interference ability, good reproducibility and stability. This set of carbon nanotubes, polyelectrolyte and noble metal nanoparticles as a whole The construction of nanocomposite provides a good research platform for high efficient and sensitive electrochemical detection of dopamine.

【學(xué)位授予單位】：長沙理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：O657.1;R446.12

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