金屬-有機(jī)框架結(jié)構(gòu)材料的制備及其在電化學(xué)生物傳感中的應(yīng)用
發(fā)布時間：2018-08-30 15:44
【摘要】：隨著科技水平的逐漸發(fā)展,腦神經(jīng)電分析化學(xué)的研究正在成為生命分析化學(xué)領(lǐng)域的熱點課題之一。腦神經(jīng)化學(xué)過程的研究是涉及分析化學(xué)、生命科學(xué)等多種學(xué)科相互交叉的前沿研究領(lǐng)域。分析化學(xué)的發(fā)展促進(jìn)了腦神經(jīng)科學(xué)的發(fā)展,同時腦神經(jīng)科學(xué)的發(fā)展也給分析化學(xué)提供了更多的機(jī)遇和挑戰(zhàn)。就反應(yīng)、傳遞、分布等方面而言,神經(jīng)化學(xué)的動態(tài)過程展現(xiàn)了神經(jīng)元與腦結(jié)構(gòu)功能的獨特性,我們需要深入挖掘生物體由復(fù)雜的神經(jīng)活動組成的神經(jīng)化學(xué)過程的本質(zhì)。中樞神經(jīng)系統(tǒng)約38億年進(jìn)化為其化學(xué)研究帶來了特殊的復(fù)雜性,神經(jīng)化學(xué)與反應(yīng)容器或其他生物化學(xué)中的純化學(xué)反應(yīng)不同,不可僅通過傳統(tǒng)的化學(xué)方法來理解。幸運的是,科學(xué)家在神經(jīng)科學(xué)的研究中取得了巨大的進(jìn)步,這是由新的微觀或納米概念和技術(shù)推動的,特別是關(guān)于定性和定量監(jiān)測活動物腦中神經(jīng)化學(xué)物質(zhì)的(近)實時變化(稱為體內(nèi)分析)。利用電化學(xué)分析方法來進(jìn)行腦神經(jīng)系統(tǒng)中神經(jīng)遞質(zhì)、調(diào)質(zhì)、能量代謝物質(zhì)、自由基等重要生理活性物質(zhì)的活體實時動態(tài)分析,在腦功能和各種腦疾病的生理和病理研究中正在發(fā)揮著重要的作用。在前人種類繁多的研究成果基礎(chǔ)上,設(shè)想利用材料方面的優(yōu)勢為活體電化學(xué)分析探索一條新的道路。本論文以近年來研究熱點之一的金屬-有機(jī)框架結(jié)構(gòu)材料為基礎(chǔ),利用其本身高孔隙率、大比表面積以及良好的可調(diào)控和可設(shè)計性的優(yōu)點,并將其或其熱解產(chǎn)物與多壁碳納米管、石墨烯或碳纖維等一系列碳材料相復(fù)合。碳材料作為復(fù)合材料的基底構(gòu)筑了材料與電極之間良好的電子傳遞通道,有效地克服了其導(dǎo)電性較差的缺點。其中,由碳纖維為基底的金屬-有機(jī)框架結(jié)構(gòu)材料或其熱解產(chǎn)物復(fù)合材料制成的微電極具有微米級尺寸,對生物體的損傷較小,且活體伏安分析法具有較高的時間和空間分辨率等特點,非常適合于腦內(nèi)生理條件下電化學(xué)活性物質(zhì)的活體分析檢測。本論文通過在不同碳材料基底上復(fù)合金屬-有機(jī)框架結(jié)構(gòu)或其熱解產(chǎn)物,制備了一系列復(fù)合材料電化學(xué)生物傳感器,并成功地對鼠腦內(nèi)一些重要的生理電化學(xué)活性物質(zhì)(5-羥色胺和氧氣等)進(jìn)行了腦神經(jīng)化學(xué)過程的電化學(xué)分析研究,主要研究內(nèi)容以及相關(guān)結(jié)論包括以下三個部分:(1)我們合成了基于碳材料(多壁碳納米管和石墨烯)的金屬-有機(jī)框架結(jié)構(gòu)(Al-MIL-53-NH2)復(fù)合材料電化學(xué)生物傳感器,通過與碳材料相結(jié)合完善了材料本身的電子傳遞途徑,有效地提高了金屬-有機(jī)框架結(jié)構(gòu)材料的導(dǎo)電性,同時利用金屬-有機(jī)框架結(jié)構(gòu)材料本身所具有的良好的多孔吸附特性,對多巴胺進(jìn)行了富集后的電化學(xué)分析檢測。結(jié)果顯示,多巴胺的氧化峰電流在一定濃度范圍內(nèi)呈現(xiàn)良好的線性關(guān)系,同時還發(fā)現(xiàn)該材料對抗壞血酸也有一定的屏蔽效果。(2)我們制備了基于金屬-有機(jī)框架結(jié)構(gòu)(UiO-66-SO3H)的碳纖維微電極電化學(xué)生物傳感器,并成功地利用其良好的富集效果檢測出鼠腦紋狀體腦區(qū)5-羥色胺的基礎(chǔ)濃度。金屬-有機(jī)框架結(jié)構(gòu)與碳纖維地結(jié)合構(gòu)建了一個良好的電子傳遞通道,有效地提高了金屬-有機(jī)框架結(jié)構(gòu)材料的導(dǎo)電能力。動物的驗證實驗強(qiáng)有力地證明了我們所檢測的腦生理電化學(xué)活性的物質(zhì)正是5-羥色胺。我們所制備的基于金屬-有機(jī)框架結(jié)構(gòu)的碳纖維復(fù)合材料微電極電化學(xué)生物傳感器具有選擇性良好,靈敏度較高的特點。(3)我們制備了基于沸石咪唑酯框架結(jié)構(gòu)(ZIF-67)熱解產(chǎn)物碳纖維微電極電化學(xué)生物傳感器。這種材料作為非貴金屬的氧還原催化劑在人工腦脊液中具有近乎四電子的良好催化效果,大大減少了兩電子還原產(chǎn)物過氧化氫的生成。同時由于其抗干擾效果很好,我們成功將其用于鼠腦海馬體腦區(qū)氧氣濃度的檢測,并對多種生理病理情況下氧氣濃度變化情況進(jìn)行實時監(jiān)測。這對于生理學(xué)與病理學(xué)的研究都具有極其重要的意義。
[Abstract]:With the development of science and technology, the study of electroencephalographic analysis chemistry is becoming one of the hot topics in the field of life analytical chemistry. The development of brain neuroscience also provides more opportunities and challenges for analytical chemistry. In terms of reaction, transmission, distribution, and so on, the dynamic processes of Neurochemistry demonstrate the uniqueness of neurons and brain structures and functions. We need to dig deeply into the nature of neurochemical processes in organisms composed of complex neural activities. The evolution of systems over the past 3.8 billion years has brought special complexity to their chemical research. Neurochemistry, unlike pure chemical reactions in reaction containers or other biochemistry, cannot be understood solely by traditional chemical methods. Fortunately, scientists have made tremendous progress in neuroscience research, which is based on new microscopic or nanoscale concepts. Technology-driven, especially for qualitative and quantitative monitoring of near-real-time (in vivo) changes in neurochemicals in the brain of living animals. In vivo dynamic analysis of neurotransmitters, modulators, energy metabolites, free radicals, and other important physiological active substances in the brain nervous system using electrochemical methods. Based on the results of previous studies, it is envisaged to explore a new way for in vivo electrochemical analysis by utilizing the advantages of materials. This paper is based on the metal-organic frameworks, which are one of the hotspots in recent years. High porosity, large specific surface area, good controllability and designability, and their pyrolysis products are compounded with a series of carbon materials, such as multi-walled carbon nanotubes, graphene or carbon fibers. Carbon materials as the substrate of composite materials construct a good electron transfer channel between materials and electrodes, and effectively overcome them. Among them, microelectrodes made of metal-organic frameworks based on carbon fibers or their pyrolysis products have the characteristics of micron size, less damage to organisms, and high time and spatial resolution in vivo voltammetry, so they are very suitable for electronics in brain physiological conditions. In this paper, a series of composite electrochemical biosensors were fabricated by using metal-organic frameworks or their pyrolysis products on different carbon substrates. Some important electrophysiological active substances (5-hydroxytryptamine, oxygen, etc.) in the rat brain were successfully neutralized. The main research contents and conclusions of the electrochemical analysis of the chemical process include the following three parts: (1) We synthesized metal-organic frameworks (Al-MIL-53-NH2) composite electrochemical biosensors based on carbon materials (multi-walled carbon nanotubes and graphene). The electrons of the materials were improved by combining with carbon materials. The conductivity of metal-organic frameworks was effectively improved by the transfer pathway, and the electrochemical analysis of dopamine was carried out by using the good porous adsorption characteristics of metal-organic frameworks. The results showed that the oxidation peak current of dopamine was good in a certain concentration range. (2) We fabricated a carbon fiber microelectrode electrochemical biosensor based on metal-organic framework (UiO-66-SO3H) and successfully detected the basal concentration of 5-hydroxytryptamine in the striatum of rat brain using its good enrichment effect. A good electron transfer channel is constructed by the combination of the frame structure and carbon fiber, which effectively improves the conductivity of the metal-organic frame structure materials. Animal experiments strongly demonstrate that the electrophysiological activity of the brain detected by us is exactly 5-hydroxytryptamine. Carbon fiber composite microelectrode electrochemical biosensor based on zeolite imidazole ester (ZIF-67) pyrolysis product was prepared. This material was used as a non-noble metal oxygen reduction catalyst in artificial cerebrospinal fluid (ACF). Because of its good anti-interference effect, we have successfully applied it to the detection of oxygen concentration in the hippocampus of rat brain and real-time monitoring of oxygen concentration changes under various physiological and pathological conditions. Pathological studies are of great importance.
【學(xué)位授予單位】：上海師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O657.1
，
本文編號：2213533
[Abstract]:With the development of science and technology, the study of electroencephalographic analysis chemistry is becoming one of the hot topics in the field of life analytical chemistry. The development of brain neuroscience also provides more opportunities and challenges for analytical chemistry. In terms of reaction, transmission, distribution, and so on, the dynamic processes of Neurochemistry demonstrate the uniqueness of neurons and brain structures and functions. We need to dig deeply into the nature of neurochemical processes in organisms composed of complex neural activities. The evolution of systems over the past 3.8 billion years has brought special complexity to their chemical research. Neurochemistry, unlike pure chemical reactions in reaction containers or other biochemistry, cannot be understood solely by traditional chemical methods. Fortunately, scientists have made tremendous progress in neuroscience research, which is based on new microscopic or nanoscale concepts. Technology-driven, especially for qualitative and quantitative monitoring of near-real-time (in vivo) changes in neurochemicals in the brain of living animals. In vivo dynamic analysis of neurotransmitters, modulators, energy metabolites, free radicals, and other important physiological active substances in the brain nervous system using electrochemical methods. Based on the results of previous studies, it is envisaged to explore a new way for in vivo electrochemical analysis by utilizing the advantages of materials. This paper is based on the metal-organic frameworks, which are one of the hotspots in recent years. High porosity, large specific surface area, good controllability and designability, and their pyrolysis products are compounded with a series of carbon materials, such as multi-walled carbon nanotubes, graphene or carbon fibers. Carbon materials as the substrate of composite materials construct a good electron transfer channel between materials and electrodes, and effectively overcome them. Among them, microelectrodes made of metal-organic frameworks based on carbon fibers or their pyrolysis products have the characteristics of micron size, less damage to organisms, and high time and spatial resolution in vivo voltammetry, so they are very suitable for electronics in brain physiological conditions. In this paper, a series of composite electrochemical biosensors were fabricated by using metal-organic frameworks or their pyrolysis products on different carbon substrates. Some important electrophysiological active substances (5-hydroxytryptamine, oxygen, etc.) in the rat brain were successfully neutralized. The main research contents and conclusions of the electrochemical analysis of the chemical process include the following three parts: (1) We synthesized metal-organic frameworks (Al-MIL-53-NH2) composite electrochemical biosensors based on carbon materials (multi-walled carbon nanotubes and graphene). The electrons of the materials were improved by combining with carbon materials. The conductivity of metal-organic frameworks was effectively improved by the transfer pathway, and the electrochemical analysis of dopamine was carried out by using the good porous adsorption characteristics of metal-organic frameworks. The results showed that the oxidation peak current of dopamine was good in a certain concentration range. (2) We fabricated a carbon fiber microelectrode electrochemical biosensor based on metal-organic framework (UiO-66-SO3H) and successfully detected the basal concentration of 5-hydroxytryptamine in the striatum of rat brain using its good enrichment effect. A good electron transfer channel is constructed by the combination of the frame structure and carbon fiber, which effectively improves the conductivity of the metal-organic frame structure materials. Animal experiments strongly demonstrate that the electrophysiological activity of the brain detected by us is exactly 5-hydroxytryptamine. Carbon fiber composite microelectrode electrochemical biosensor based on zeolite imidazole ester (ZIF-67) pyrolysis product was prepared. This material was used as a non-noble metal oxygen reduction catalyst in artificial cerebrospinal fluid (ACF). Because of its good anti-interference effect, we have successfully applied it to the detection of oxygen concentration in the hippocampus of rat brain and real-time monitoring of oxygen concentration changes under various physiological and pathological conditions. Pathological studies are of great importance.
【學(xué)位授予單位】：上海師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O657.1
，
本文編號：2213533
本文鏈接：http://sikaile.net/kejilunwen/huaxue/2213533.html
最近更新
教材專著
