本文選題：碳納米管 + 石墨烯��； 參考：《大連理工大學》2015年碩士論文

【摘要】：發(fā)展水體中痕量污染物的檢測方法對于保障水體質(zhì)量和公共衛(wèi)生意義重大�；趥鞲衅鞯臋z測方法有響應快速、靈敏度高、易于操作等諸多優(yōu)點,在環(huán)境污染物的現(xiàn)場檢測方面有著巨大的潛力。近年來,碳納米管和石墨烯由于優(yōu)異的光學、電學等特性,在傳感器領域獲得了廣泛的應用。本論文分別構建了基于單壁碳納米管和石墨烯的電阻傳感器,用于水體中微囊藻毒素-LR (MC-LR)和雙酚A(BPA)的檢測。具體內(nèi)容如下：采用光刻和磁濺射工藝在SiO2/Si表面制備了金叉指電極。利用氨丙基三乙氧基硅烷(APTES)對金叉指電極進行修飾。然后成功將單壁碳納米管(SWCNTs)沉積在金叉指電極表面,構建了CNT電阻傳感器。掃描電鏡(SEM)表明,CNT在金叉指電極溝道內(nèi)形成均勻、致密的網(wǎng)絡,可以作為傳感器導電的溝道。為檢測MC-LR,首先把MC-LR固定到SWCNTs修飾的金叉指電極上,再接著連接上抗MC-LR單克隆抗體。新加入的MC-LR樣品通過競爭鍵合作用誘導SWCNTs上抗體-抗原復合物的抗體分離,這導致傳感器的電導發(fā)生變化。無標記的免疫傳感器對取以10為底的濃度在1-1000 ng/L的MC-LR有著廣泛的線性響應,檢測限為0.6 ng/L。將該傳感器用于添加MC-LR的自來水、河水和湖泊水樣品的分析,回收率分別為96.5～112.6%,102.2～124.2%和84.7～104.7%,相對標準偏差(RSDs)為9.1～18.7%。將單層氧化石墨烯(GO)沉積在APTES功能化的金叉指電極表面,利用單線性掃描伏安法(LSV)對電極表面的GO進行電化學還原,然后在250℃空氣氛圍下熱退火。SEM分析表明,沉積的GO均勻覆蓋在金叉指電極表面,形成了傳感器導電的溝道。拉曼分析和電化學測量表明,十次單線性掃描伏安掃描和熱退火可將傳感器的電阻進一步降低。為檢測BPA,我們選擇了對BPA具有特異性識別的單鏈DNA適配子(序列：(5'-(NH2C3)CCGGTGGGTGGTCAGGTGGGATAGCGTTCCGCGTATGGCCCAGCGC ATCACGGGTTCGCACCA-3'),適配子會通過物理吸附方式附著在還原的GO表面。同時考察了DNA適配子濃度的影響,結(jié)果表明,使用500 nmol/L的DNA適配子進行修飾可以獲得最佳的響應特性。免疫電阻傳感器對濃度在1-500 nmol/L BPA有著線性的響應,檢測限為0.7 nmol/L。將該傳感器用于添加BPA的河水和自來水樣品的分析,回收率分別為82.7～92.8%和102.2～120.1%,相對標準偏差(RSDs)為9.2～20.7%。
[Abstract]:It is of great significance to develop the detection method of trace pollutants in water body to ensure water quality and public health. The detection method based on sensor has many advantages, such as fast response, high sensitivity, easy to operate and so on, so it has great potential in the field detection of environmental pollutants. In recent years, carbon nanotubes and graphene have been widely used in sensor field due to their excellent optical and electrical properties. In this paper, resistance sensors based on single-walled carbon nanotubes and graphene were constructed for the detection of microcystin-LR (MC-LR) and bisphenol A (BPA) in water. The main contents are as follows: gold finger electrode was fabricated on SiO2/Si surface by photolithography and magnetron sputtering. The gold interDigital electrode was modified with aminopropyl triethoxy silane (APTES). Then the single walled carbon nanotubes (SWCNTs) were successfully deposited on the surface of the gold finger electrode and the CNT resistor sensor was constructed. Scanning electron microscopy (SEM) showed that CNT formed a uniform and dense network in the channel of the gold finger electrode and could be used as the conductive channel of the sensor. In order to detect MC-LRs, MC-LR was first immobilized on the gold finger electrode modified by SWCNTs, and then the monoclonal antibody against MC-LR was attached. The newly added MC-LR samples are separated by competitive bonding to induce antibody separation of the antibody-antigen complex on SWCNTs, which results in the change of the conductivity of the sensor. The unlabeled immunosensor has a broad linear response to MC-LR with a concentration of 10 to 1-1000 ng/L, with a detection limit of 0.6 ng / L. The sensor was applied to the analysis of tap water, river water and lake water with MC-LR. The recoveries of the sensor were 96.5 ~ 112.6% and 84.7% ~ 104.2%, respectively, and the relative standard deviation (RSD) was 9.1 ~ 18.7%. Single layer graphene oxide (GOO) was deposited on the surface of APTES functionalized gold finger electrode. Go on the electrode surface was reduced by single linear scanning voltammetry. The deposited go is uniformly covered on the surface of the gold finger electrode, forming a channel for conducting the sensor. Raman analysis and electrochemical measurements show that the resistance of the sensor can be further reduced by single linear scanning voltammetry and thermal annealing. In order to detect the BPA, we selected a single-stranded DNA adaptor (sequence: 5) -NH2C3 / CCGGTGGGGGGGATAGTAGTAGTTCCGTAGGGGC ATCACGGGGTTCGCACCA-3, which is attached to the reduced go surface by physical adsorption. At the same time, the effect of DNA adaptor concentration was investigated. The results show that the best response characteristics can be obtained by modifying 500 nmol/L DNA adaptor. The immunoresistive sensor has a linear response to the concentration of 1-500 nmol/L BPA, with a detection limit of 0.7 nmol / L. The sensor was applied to the analysis of water and tap water samples with BPA. The recoveries were 82.7% and 102.2%, respectively. The relative standard deviation (RSDs) was 9.2% and 20.7%, respectively.
【學位授予單位】：大連理工大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：X830;TP212

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本文編號：1870383