【摘要】：石墨烯是一種二維(2D)周期性蜂窩狀點(diǎn)陣結(jié)構(gòu),平面由碳六元環(huán)組成的,通過不同的方式,如卷曲,翹曲或堆積,可以形成零維(0D)的富勒烯(fullerene),一維(1D)的碳納米管(carbon nano-tube,CNT)或者三維(3D)的石墨(graphite)。作為一種新型2D平面碳材料,石墨烯因?yàn)榫哂袃?yōu)異力學(xué)、熱學(xué)、光學(xué)、電學(xué)性能而受到外界的廣泛關(guān)注。而石墨烯特殊的結(jié)構(gòu)也使其在電化學(xué)領(lǐng)域有廣泛應(yīng)用。基于石墨烯衍生物——氧化石墨烯(GO)還原得到的石墨烯(rGO)具有良好的導(dǎo)電性,且表面含有少量功能基團(tuán),是一種理想的電化學(xué)電極材料。另外,GO易于分散、表面修飾且生物相容性良好,在細(xì)胞調(diào)控和電化學(xué)生物傳感器構(gòu)筑方面具有獨(dú)特的優(yōu)勢。而為滿足特殊環(huán)境和人體特殊構(gòu)造測試需要,開發(fā)新型的,高品質(zhì)的柔性器件越來越受到人們的關(guān)注。柔性傳感器是柔性器件非常重要的組件,傳感器的性能直接決定了柔性器件的性能。隨著柔性器件得到越來越廣泛的應(yīng)用,開發(fā)出基于石墨烯的柔性傳感器件,成為眾多研究學(xué)者共同努力的方向。與剛性基底相比,基于石墨烯高柔韌性和機(jī)械強(qiáng)度,制備的石墨烯柔性電極,可以使電極與靶組織良好接觸,減少電極和組織之間的機(jī)械強(qiáng)度的不匹配,可以減少臨床應(yīng)用中產(chǎn)生的機(jī)械損傷和免疫反應(yīng)。因此受到廣泛關(guān)注。本文分別采用軟光刻轉(zhuǎn)印技術(shù)和紫外光刻微加工技術(shù)在不同剛性基底上構(gòu)筑了圖案化的GO陣列和GO/rGO微陣列。探究了神經(jīng)細(xì)胞PC12在不同剛性基底表面選擇性粘附以及其在GO/rGO微陣列表面粘附、增殖的行為。深入研究GO/rGO圓盤陣列電極在不同彎曲曲率下的電化學(xué)特性,并對PC12細(xì)胞釋放物(雙氧水H2O2)進(jìn)行檢測。具體研究內(nèi)容如下:1、利用軟光刻微接觸印刷技術(shù),以表面具有微結(jié)構(gòu)的聚二甲基硅氧烷(PDMS)為轉(zhuǎn)移印章,在不同剛性基底表面制備圖案化GO薄膜。通過調(diào)節(jié)旋涂GO溶液的次數(shù)和旋涂轉(zhuǎn)速控制成膜質(zhì)量。著重探究了印章表面(0.36cm2)施加不同壓力(0.10N、0.20N、0.25N、0.35N、0.45N、0.50N、0.55N、1N)時(shí)對成膜質(zhì)量的影響。研究結(jié)果表明,印章表面施加壓力為0.5N,維持12h時(shí)得到比較均勻規(guī)整的GO圖案,厚度約10nm。GO表面含有豐富的官能團(tuán),具有很好的親水性,便于細(xì)胞粘附增殖。在不同剛性基底表面轉(zhuǎn)印GO陣列并接種PC12細(xì)胞,發(fā)現(xiàn)神經(jīng)細(xì)胞更傾向于粘附在剛度較小的GO陣列表面。2、通過微加工工藝和電化學(xué)還原技術(shù),在柔性基底上制備了與光刻尺寸相匹配的GO/rGO微陣列。對微陣列表面形貌及微觀結(jié)構(gòu)進(jìn)行了表征。研究不同形狀、不同尺寸微圖案對PC12細(xì)胞粘附、增殖行為的影響。研究發(fā)現(xiàn),GO/rGO微陣列表面接種細(xì)胞后,細(xì)胞更傾向于粘附在GO表面,并沿著GO/rGO邊界生長延伸。這種行為有利于細(xì)胞受到藥物刺激釋放的活性物質(zhì)迅速擴(kuò)散到電極表面。3、探究了不同曲率下微陣列電極電化學(xué)特性的變化規(guī)律。研究結(jié)果表明,借助循環(huán)伏安測試方法優(yōu)選的微陣列電極的最佳尺寸為直徑20μm、間距60μm的圓盤陣列。在0.6V條件下,微陣列電極表現(xiàn)出良好的催化氧化H2O2的性能,實(shí)現(xiàn)了材料表面無任何催化劑修飾不同曲率條件下對低含量H2O2的檢測。實(shí)施藥物刺激后,不同曲率的陣列電極對細(xì)胞釋放的活性物質(zhì)H2O2的響應(yīng)程度不同。相同條件下,電極向內(nèi)彎(曲率k0)時(shí),隨著曲率的增大,電極檢測性能得到提升;而電極外彎(曲率k0)時(shí),隨曲率增加,測定結(jié)果基本相同。出現(xiàn)這種結(jié)果的原因是由于內(nèi)彎時(shí)陣列電極附近,電勢線密度增加,電場強(qiáng)度增強(qiáng),細(xì)胞跨膜電壓增大,從而提升微陣列電極的電化學(xué)催化活性。
[Abstract]:Graphene is a two-dimensional (2D) periodic honeycomb lattice structure consisting of carbon six-membered rings, such as curling, warping or stacking, can form a zero dimension (0D) fullerene, one-dimensional (1D) carbon nanotubes, cnts) or three-dimensional (3d) graphite. As a novel 2D planar carbon material, graphene is attracted to the outside world due to its excellent mechanical, thermal, optical and electrical properties. and the special structure of graphene has wide application in the field of electrochemistry. Graphene (rGO) obtained by reduction of graphene derivative _ graphene oxide (GO) has good conductivity, and a small amount of functional groups on the surface is an ideal electrochemical electrode material. In addition, GO is easy to disperse, has good surface modification and good biocompatibility, and has unique advantages in cell regulation and electrochemical biosensor construction. In order to meet the needs of special environment and special structural test of human body, the development of new and high-quality flexible devices has attracted more and more attention. A flexible sensor is a very important component of a flexible device, and the performance of the sensor directly determines the performance of the flexible device. With the more and more extensive application of flexible devices, graphene-based flexible sensor has been developed, which has become the direction of joint efforts of many researchers. Compared with the rigid substrate, the graphene flexible electrode prepared based on the high flexibility and mechanical strength of the graphene can make the electrode contact with the target tissue in good contact, so that the mismatching of mechanical strength between the electrode and the tissue can be reduced, and mechanical damage and immune reaction generated in clinical application can be reduced. As a result, extensive attention has been given. In this paper, a patterned GO array and GO/ rGO micro-array were constructed on different rigid substrates by soft lithography transfer and UV lithography. The selective adhesion of PC12 cells on different rigid substrates and the adhesion and proliferation of PC12 cells on the surface of GO/ rGO microarray were investigated. The electrochemical properties of GO/ rGO disk array electrodes under different bending curvature were studied, and the release of PC12 cells (H2O2) was investigated. The specific research contents are as follows: 1. Using soft lithography micro-contact printing technology, a patterned GO film is prepared on different rigid substrate surfaces by using polydimethylsiloxane (PDMS) with micro structure as transfer seal. The film forming quality is controlled by adjusting the number of spin coating GO solutions and the spin coating speed. The influences of different pressures (0. 10N, 0. 20N, 0. 25N, 0. 35N, 0. 45N, 0. 50N, 0. 55N, 1N) on the film forming quality were investigated. The results show that the pressure on the surface of the seal is 0. 5N. When maintaining 12h, the uniform and regular GO pattern is obtained. The thickness is about 10nm. The GO surface contains rich functional groups, has good hydrophilicity, and is convenient for cell adhesion and proliferation. After the transfer of GO arrays on the surface of different rigid substrates and inoculation of PC12 cells, it was found that nerve cells were more likely to adhere to the lower stiffness GO array surface. 2. The GO/ rGO microarray matching the lithography dimension was prepared on the flexible substrate by micro-processing and electrochemical reduction techniques. The surface morphology and microstructure of microarray were characterized. The effects of different shapes and micro patterns on adhesion and proliferation of PC12 cells were studied. It was found that after inoculation of cells on the surface of GO/ rGO microarray, cells tended to adhere to the GO surface and extend along the GO/ rGO boundary. This behavior is beneficial to the rapid diffusion of the active substance released by drug stimulation to the surface of the electrode. The results show that the optimal size of the microarray electrode is 20. m u.m in diameter and 60. m u.m in pitch by means of cyclic voltammetry. Under the condition of 0. 6V, the microarray electrode showed good catalytic oxidation of H2O2 and realized the detection of low content of H2O2 under different curvature conditions without any catalyst modification on the surface of the material. After drug stimulation, the degree of response of the array electrodes of different curvatures to the active substance H2O2 released by the cells was different. In the same condition, when the electrode bends inward (curvature k0), as the curvature increases, the electrode detection performance is improved; and when the electrode outer bend (curvature k0) increases with the curvature, the measurement result is substantially the same. This result is due to increased potential line density, increased electric field strength, increased cell cross-membrane voltage, and enhanced electrochemical catalytic activity of microarray electrodes due to the increase in potential line density near the array electrodes at the time of internal bending.
【學(xué)位授予單位】：浙江理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O613.71;O657.1

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