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基于離子液體基鉑納米流體電化學(xué)傳感器的構(gòu)建及其應(yīng)用研究

發(fā)布時(shí)間:2019-05-14 12:11
【摘要】:納米流體自被提出后廣受關(guān)注,不同基質(zhì)的納米流體如水基、油基、液體石蠟基等不斷被合成,并在生物醫(yī)學(xué)、催化、制冷等方面得到不斷應(yīng)用。傳統(tǒng)的納米流體介質(zhì)多為水、有機(jī)溶劑以及油,然而此類溶劑的熱穩(wěn)定性較差,揮發(fā)后對(duì)環(huán)境和人體健康造成影響。離子液體具有納米流體介質(zhì)所需的導(dǎo)熱性和熱穩(wěn)定性,是名副其實(shí)的綠色溶劑,同時(shí)能夠作為模板劑實(shí)現(xiàn)對(duì)無機(jī)納米材料結(jié)構(gòu)的控制,可以對(duì)納米粒子進(jìn)行表面修飾從而有效阻止納米粒子團(tuán)聚,這些特性為納米流體的合成提供了新契機(jī)。本實(shí)驗(yàn)探索了在1-丁基-3-甲基咪唑四氟硼酸為介質(zhì),以離子液體中的聚乙烯基吡咯烷酮(PVP)為萃取劑,將水相中的[Pt Cl4]2-萃取到離子液體相中。在超聲輔助條件下用硼氫化鈉將離子液體相中的鉑離子還原,制備了親水性離子液體基鉑納米流體。同時(shí)對(duì)合成條件、納米顆粒的形貌及穩(wěn)定性進(jìn)行了探討。離子液體有寬電化學(xué)窗口和良好的導(dǎo)電性,納米流體具有較好的導(dǎo)電性和高電催化活性,以離子液體為基質(zhì)合成離子液體基納米流體在電化學(xué)傳感領(lǐng)域有著廣闊的應(yīng)用。本實(shí)驗(yàn)著重探討了離子液體基鉑納米流體修飾電極構(gòu)建電化學(xué)傳感器用于尿酸、抗壞血酸和多巴胺的單組份和多組分測(cè)定,探索了離子液體基鉑納米流體在電分析化學(xué)領(lǐng)域的應(yīng)用。本論文主要研究的內(nèi)容和結(jié)果如下:1、[BMIm]BF4離子液體為介質(zhì),在1-丁基-3-甲基咪唑四氟硼酸/硫酸銨雙水相體系中,聚乙烯吡咯烷酮(PVP)作萃取劑、穩(wěn)定劑,在超聲條件下制備1-丁基-3-甲基咪唑四氟硼酸鉑納米流體(Pt-[BMIm]BF4),同時(shí)用納米粒度儀、透射電子顯微鏡、傅里葉紅外光譜儀等對(duì)納米流體進(jìn)行表征。結(jié)果表明,制備的鉑納米流體中鉑納米顆粒平均粒度在31.2nm左右,且分布均勻、大小均一、穩(wěn)定性好。PVP不僅阻止了納米粒子間的團(tuán)聚,還增強(qiáng)了鉑納米粒子的抗氧化性,獲得了穩(wěn)定的離子液體基鉑納米流。2、用離子液體基鉑納米流體(ILPtNFs)為修飾材料,制備電化學(xué)傳感器,構(gòu)建了測(cè)定多巴胺(DA)、尿酸(UA)、抗壞血酸(AA)的電化學(xué)傳感器。采用循環(huán)伏安法研究了DA、UA、AA在該修飾電極上的電化學(xué)行為,以差示脈沖伏安法(DPV)建立了單獨(dú)測(cè)定DA、UA、AA含量的方法。實(shí)驗(yàn)表明,分別在pH=3.0、pH=6.0和pH=6.0的磷酸緩沖溶液(PBS)中,ILPtNFs對(duì)AA、DA和UA具有明顯的電催化作用。在最佳的實(shí)驗(yàn)條件下,DA氧化峰電流與其濃度在8.0×10-6-4.0×10-4 mol/l范圍內(nèi)呈良好的線性關(guān)系。UA氧化峰電流與其濃度在2.0×10-6-1.0×10-4 mol/l范圍內(nèi)呈良好的線性關(guān)系。AA氧化峰電流與其濃度在2.0×10-6-1.0×10-4 mol/l范圍內(nèi)呈良好的線性關(guān)系。將該方法分別用于鹽酸多巴胺注射液中DA含量、人體尿液中UA含量、維生素C注射液中AA含量的測(cè)定,結(jié)果滿意。3、滴涂法將ILPtNFs固定至玻碳電極表面制備電化學(xué)傳感器,以差示脈沖伏安法(DPV)建立同時(shí)測(cè)定UA、DA和AA混合液的新方法。實(shí)驗(yàn)結(jié)果顯示,ILPtNFs修飾電極能實(shí)現(xiàn)DA、UA和AA的良好分離。在實(shí)驗(yàn)優(yōu)化條件下,當(dāng)濃度在4.0×10-6 1.0×10-4 mol/l范圍內(nèi)時(shí),分別改變UA、DA和AA的濃度,三者的峰電流與濃度呈良好的線性關(guān)系;同時(shí)改變UA、DA和AA的濃度,三者的峰電流與濃度呈良好的線性關(guān)系。該方法可用于實(shí)際樣品中UA、DA和AA的定量檢測(cè),結(jié)果滿意。
[Abstract]:The nano-fluid has been widely concerned since being put forward, and the nano-fluids of different substrates, such as water-based, oil-based, liquid paraffin, and the like, are continuously synthesized, and are continuously applied in the fields of biomedicine, catalysis, refrigeration and the like. The traditional nano-fluid medium is water, an organic solvent and oil, however, the thermal stability of such a solvent is poor, and the environment and the health of the human body are affected after volatilization. the ionic liquid has the thermal conductivity and the thermal stability required by the nano fluid medium, is a veritable green solvent, can be used as a template agent to control the structure of the inorganic nano material, These properties provide a new opportunity for the synthesis of nanofluids. In this experiment, the aqueous phase of[Pt _ 4] 2-in the aqueous phase was extracted into the ionic liquid phase with 1-butyl-3-methylcyclotetrafluoro-boric acid as the medium, and the polyethylene-based polyoxyalkanone (PVP) in the ionic liquid was used as the extractant. A hydrophilic ionic liquid-based platinum nano-fluid is prepared by reducing the platinum ions in the ionic liquid phase with sodium borohydride under the ultrasonic-assisted conditions. The morphology and stability of the nano-particles were also discussed. The ionic liquid has wide electrochemical window and good electrical conductivity, the nano fluid has good electrical conductivity and high electrocatalytic activity, and the ionic liquid is used as the matrix to synthesize the ionic liquid-based nano fluid and has wide application in the field of electrochemical sensing. The application of the ionic liquid-based platinum nano-fluid in the field of electroanalytical chemistry is discussed. The main contents and results of this thesis are as follows:1,[BMIm] BF4 ionic liquid is the medium, in the 1-butyl-3-medetomidine tetrafluoboric acid/ sulfuric acid aqueous two-phase system, the polyethylene and the alkanone (PVP) are used as the extractant and the stabilizer, 1-butyl-3-methyl-4-fluoroborate (Pt-[BMIm] BF4) was prepared under ultrasonic conditions, and the nano-fluid was characterized by a nano-particle size instrument, a transmission electron microscope, a Fourier transform infrared spectrometer, and the like. The results show that the average particle size of the platinum nanoparticles in the prepared platinum nano-fluid is about 31.2 nm, the distribution is uniform, the size is uniform, and the stability is good. The PVP not only prevents the agglomeration of the nano-particles, but also enhances the oxidation resistance of the platinum nano-particles, and obtains a stable ionic liquid-based platinum nano-flow.2, using the ionic liquid-based platinum nano-fluid (ILPtNFs) as a modified material, preparing an electrochemical sensor, and constructing a dopamine (DA), Electrochemical sensors for uric acid (UA), ascorbic acid (AA). The electrochemical behavior of DA, UA and AA on the modified electrode was studied by cyclic voltammetry, and the method of separately measuring the content of DA, UA and AA was established by differential pulse voltammetry (DPV). The results showed that ILPNFs had a significant electrocatalytic effect on AA, DA and UA in phosphate buffer (PBS) with pH = 3.0, pH = 6.0 and pH = 6.0, respectively. Under the best experimental conditions, the peak current of DA is in good linear relationship with its concentration in the range of 8.0-10-6-4.0-10-4mol/ l. The UA oxidation peak current has a good linear relationship with its concentration in the range of 2.0-10-6-1.0-10-4mol/ l. The peak current of AA is in a good linear relationship with its concentration in the range of 2.0-10-6-1.0-10-4mol/ l. The method is used for the determination of the content of DA in the dopamine injection of the hydrochloric acid, the content of the UA in the urine of the human body, the content of the AA in the vitamin C injection, and the result is satisfied. A new method for simultaneous determination of the mixture of UA, DA and AA was established by differential pulse voltammetry (DPV). The results show that the modified electrode of ILPNFs can realize the good separation of DA, UA and AA. 鍦ㄥ疄楠屼紭鍖栨潯浠朵笅,褰撴祿搴﹀湪4.0脳10-6 1.0脳10-4 mol/l鑼冨洿鍐呮椂,鍒嗗埆鏀瑰彉UA,DA鍜孉A鐨勬祿搴,

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