【摘要】：糖尿病因能引起身體多系統(tǒng)的損害而成為威脅全球人類(lèi)健康的疾病之一。糖尿病患者在日常生活中,需要長(zhǎng)期規(guī)律地監(jiān)控血糖濃度從而降低持續(xù)高血糖引起的并發(fā)癥發(fā)病幾率,因此研發(fā)高效、可靠的葡萄糖傳感器非常重要。目前,市售的血糖儀為酶基葡萄糖電化學(xué)傳感器,該類(lèi)傳感器所使用試紙的活性物質(zhì)為葡萄糖氧化酶,酶作為價(jià)格昂貴的生物活性分子且固定化過(guò)程復(fù)雜使得該類(lèi)傳感器的成本頗高,因此人們嘗試用各種金屬及碳材料等構(gòu)建價(jià)格低廉、穩(wěn)定性好的無(wú)酶葡萄糖電化學(xué)傳感器,以期替代酶基葡萄糖電化學(xué)傳感器。近些年,有部分研究工作致力于將金屬有機(jī)骨架化合物(MOFs)用作硬模板或前驅(qū)體,以制備具有優(yōu)異電催化氧化葡萄糖活性的MOFs衍生材料。但此類(lèi)材料大多為粉體,需采用粘結(jié)劑將其涂覆于傳統(tǒng)電極上制備成工作電極,導(dǎo)致制備復(fù)雜、電活性材料易脫落、穩(wěn)定性也較差。鑒于此,本論文以泡沫鎳為基材,利用水熱合成法,在其上原位生長(zhǎng)了Ni-MOF,并以此為模板制備出自支撐的Ni@C納米片電極及CuNi@C電極,將其用于構(gòu)建無(wú)酶葡萄糖傳感器并對(duì)其性質(zhì)進(jìn)行研究。以下為本論文的主要研究結(jié)果:(1)通過(guò)水熱合成、熱解兩個(gè)步驟制備了自支撐Ni@C納米片電極,該電極具有三維多級(jí)孔道結(jié)構(gòu),在葡萄糖的無(wú)酶檢測(cè)方面表現(xiàn)出優(yōu)異的電催化活性。研究結(jié)果顯示,該電極檢測(cè)葡萄糖的靈敏度高達(dá)32.7944 mA·mM-1·cm-2,明顯優(yōu)于某些鎳基材料電極,線性范圍為0.15μmol·L-1~1.475 mmol·L-1,檢出限低至50nmol·L-1,并且該電極對(duì)葡萄糖表現(xiàn)出良好的選擇性,且具有較好的重現(xiàn)性、長(zhǎng)期穩(wěn)定性及抗氯離子毒化性能。此外,研究結(jié)果顯示自支撐Ni@C納米片電極可用于人體血清樣品的實(shí)際檢測(cè),并且測(cè)定結(jié)果具有較高的準(zhǔn)確度和精密度。(2)在自支撐Ni@C納米片電極的基礎(chǔ)上,通過(guò)恒電位電沉積的方法制備了自支撐CuNi@C電極,Cu納米顆粒均勻生長(zhǎng)于電極表面,由于Cu與Ni之間的協(xié)同催化作用,該電極具有優(yōu)異的無(wú)酶葡萄糖傳感性能。研究結(jié)果顯示該電極檢測(cè)葡萄糖的靈敏度高達(dá)17.1203 mA·mM-1·cm-2,線性范圍為0.2μmol·L-1~2.7206mmol·L-1,檢出限為66.67 nmol·L-1,電極對(duì)葡萄糖具有良好的選擇性,且表現(xiàn)出較好的重現(xiàn)性、長(zhǎng)期穩(wěn)定性和抗氯離子毒化性能,在人體血清樣品的檢測(cè)中能夠獲得與醫(yī)院檢測(cè)報(bào)告相近的結(jié)果,表明該電極具有實(shí)際應(yīng)用價(jià)值。
[Abstract]:Diabetes has become one of the diseases that threaten human health worldwide because it can cause damage to many systems. In order to reduce the incidence of complications caused by sustained hyperglycemia, it is very important to develop an efficient and reliable glucose sensor in the daily life of diabetic patients. At present, the blood glucose instrument on the market is an enzyme based glucose electrochemical sensor, and the active substance of the test paper used in this kind of sensor is glucose oxidase. Enzyme is an expensive bioactive molecule and the immobilization process is very complicated, so people try to use various metal and carbon materials to construct low price and good stability enzyme free glucose electrochemical sensor. In order to replace the enzyme-based glucose electrochemical sensor. In recent years, some researches have been devoted to the preparation of MOFs derivatives with excellent electrocatalytic oxidation of glucose by using organometallic skeleton compound (MOFs) as a hard template or precursor. However, most of these materials are powder, which need to be coated with binder on the traditional electrode to prepare working electrode, which leads to complex preparation, easy to fall off the electrically active material and poor stability. In view of this, Ni-MOF, was grown in situ by hydrothermal synthesis with nickel foam as the substrate and used as a template to prepare self-supported Ni@C nanochip electrode and CuNi@C electrode. It was used to construct enzyme-free glucose sensor and its properties were studied. The main results are as follows: (1) Self-supporting Ni@C nanochip electrode was prepared by hydrothermal synthesis and pyrolysis. The electrode has a three-dimensional multilevel pore structure and has excellent electrocatalytic activity in the non-enzymatic detection of glucose. The results show that the sensitivity of the electrode for glucose detection is as high as 32.7944 mA mM-1 cm-2, and the linear range is 0.15 渭 mol L ~ (-1) ~ 1.475 mmol ~ (-1). The detection limit is as low as 50nmol L ~ (-1), and the electrode has good selectivity for glucose. It also has good reproducibility, long-term stability and anti-chlorine poisoning property. In addition, the results show that the self-supporting Ni@C nanochip electrode can be used for the actual detection of human serum samples, and the determination results have high accuracy and precision. (2) based on the self-supporting Ni@C nanoscale electrode, Self-supporting CuNi@C electrode was prepared by potentiostatic electrodeposition. Cu nanoparticles grew uniformly on the surface of the electrode. Because of the synergistic catalysis between Cu and Ni, the electrode had excellent enzymatic glucose sensing performance. The results showed that the sensitivity of the electrode for glucose detection was as high as 17.1203 mA mM-1 cm-2, the linear range was 0.2 渭 mol L-1~2.7206mmol L -1, and the detection limit was 66.67 nmol L -1. The electrode had good selectivity for glucose, and showed good reproducibility, long-term stability and resistance to chloride poisoning. The results obtained in the detection of human serum samples are similar to those reported in hospitals, indicating that the electrode has practical application value.
【學(xué)位授予單位】：哈爾濱工業(yè)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類(lèi)號(hào)】：R587.1;O657.1

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