臺灣博碩士論文加值系統

去氧核醣核酸 (DNA) 為自然界中一維的奈米線，其獨特的自組裝性常被應用於生物感測器，以及奈米導線模版的製作。然而其不佳的電導特性，則限制了 DNA 在分子元件發展與應用的潛能。在本研究中，我們將二價鎳離子於鹼性環境下，參雜入 DNA 分子的雙股螺旋中，形成 nickel DNA (Ni-DNA)。並藉由導電掃描探針顯微鏡，及電化學分析結果可知，Ni-DNA 的導電度較原本的 DNA 有大幅的改善。其電荷可能藉由Ni-DNA中，具有良好堆疊之鹼基對間的交互作用來作傳輸，而參雜在其中的鎳離子猶如存在於 DNA 分子中的電洞，使得電子更容易利用電子跳躍 (Electron hopping) 來做電荷的傳輸，並且在鹼基上電子最高填滿軌域 (HOMO) 與最低未填滿軌域 (LUMO) 之間的能隙也因鎳離子的參雜而降低。並且由電化學的分析中可知，DNA 分子中鹼基對的堆疊，對於電荷於 Ni-DNA 中的傳輸有顯著的影響。當鹼基對的堆疊產生變化時 (例如在序列中鹼基對發生錯誤配對，即造成 �� 軌域堆疊的扭曲)，即使得電荷於 Ni-DNA 中的傳輸受到阻礙而呈現出較高的電阻值。藉由電荷於 Ni-DNA 中的傳輸特性，我們成功的將 Ni-DNA 導入至 DNA 生物感測器上的應用。對於 DNA 分子 序列中是否有鹼基對錯誤配對的情況，可以有效的檢測。並對於單一核�˙藻h型性(single nucleotide polymorphisms; SNPs) 的檢測提供了一個新的方向。
除此之外，Ni-DNA 還可以應用於固態的奈米電子元件上。在本研究中，我們將Ni-DNA 架於兩電極上，並經由電性量測的結果可知，參雜於 Ni-DNA 中的鎳離子會因電位的變化而產生氧化還原反應，此反應會使得 Ni-DNA 的電性上表現出負微分電阻的特性 (Negative differential resistance，NDR)。因此 Ni-DNA 具有極佳的電性分子元件之應用性。

DNA is a one-dimensional nanowire in nature, and it may not be used in nanodevices due to its low conductivity. In order to improve the conducting property of DNA, divalent nickel ions (Ni2+) are incorporated into the base pairs of DNA at pH ≧ 8.5 and nickel DNA (Ni-DNA) is formed. Meanwhile, electrochemical analyses by cyclic voltammetry and AC impedance show that the conductances of Ni-DNAs are better than that of native DNA by a factor of approximately 20 folds. UV spectroscopy and DNA base pair mismatch analyses of Ni-DNA show that electrons hoping through the ���{�� stacking of DNA base pairs may play a vital role for charge transport within Ni-DNA molecules. Meanwhile, the change in resistance that is caused by the mismatched of DNA can also be monitored by electrochemical. In this study, resistance increased exponentially with the number of mismatches. Accordingly, an intuitive and direct method for evaluating the numbers of DNA mismatches can possibly be achieved. Additionally, the exponential increase in the electrical resistance of mismatched Ni-DNA maybe caused by electron tunneling through the mismatch-induced potential barrier in Ni-DNA.
In addition, a molecular device that is composed of Ni-DNA molecules exhibits a negative differential resistance (NDR) behavior. When two gold electrodes were connected by Ni2+-chelated DNA (Ni-DNA) molecules which were converted from ��-DNA, not only the conductivity of DNA molecules were improved, but also an NDR device was formed at room temperature, in an ambient environment. Such NDR characteristics of a Ni-DNA device may have been caused by the redox reactions of Ni ions. This finding provides a highly potential for constructing electrical nano-devices from biological molecules. This biomaterial is a unique and designable one-dimensional bio-polymer for usage in biosensiors and nanodevices.

摘要 I
ABSTRACT II
誌謝 III
目錄 IV
表目錄 VII
圖目錄 VIII
第一章 緒論 1
1.1 前言 1
1.2 研究動機與目的 1
第二章 文獻回顧 4
2.1 DNA 簡介 4
2.1.1 去氧核醣核�˙� 4
2.1.2 DNA 一級結構 5
2.1.3 DNA 二級結構 6
2.1.4 DNA 分子的光學特性 7
2.1.5 DNA分子的電子特性 8
2.1.6 DNA 分子的導電機制 11
2.1.6.1 超交換作用 (Superexchange model) 11
2.1.6.2 電荷跳躍 (Hopping modle) 12
2.2 M-DNA 簡介 13
2.2.1 金屬離子在 DNA 分子上的配位位置 13
2.2.2 M-DNA 的基本結構和特性 14
2.2.3 M-DNA helix的電荷傳輸特性 15
2.3 分子自組裝 (Self-assembly) 特性 16
2.3.1 分子自組裝種類 16
2.3.2 自組裝單分子層 [烷基硫醇 (RSH)] 16
2.4 電化學簡介 18
2.4.1 電化學反應系統 19
2.4.2 影響電化學反應系統的因素 21
2.4.3 電極動力學[76,78] 22
2.4.4 循環伏安分析法 (Cyclic Voltarmmetry，CV) 23
2.4.4.1 可逆系統 (Reversible System) 25
2.4.4.2 不可逆系統 (Irreversible System) 26
2.4.4.3 近可逆系統 (Quasi-reversible System) 26
2.4.5 交流阻抗分析法 (Alternating Current Impedance，AC) 26
2.4.6 等效電路 26
2.5 石英晶體微量天平分析法 29
2.6 電泳分析法 30
2.7 負微分電阻 (Negative differential resistance，NDR) 31
第三章 利用電化學法分析 DNA 與 M (Ni)-DNA 的導電特性 33
3.1 前言 33
3.2 實驗 34
3.2.1 實驗藥品、溶液配製與設備 34
3.2.2 實驗操作步驟 38
3.2.2.1 Ni-DNA 的置換 38
3.2.2.2 紫外光與可見光吸收光譜分析 38
3.2.2.3 電泳分析 38
3.2.2.4 金電極表面清洗 38
3.2.2.5 石英晶體微量天平分析 39
3.2.2.6 導電掃描探針顯微鏡分析 39
3.2.2.7 電化學系統 40
3.2.2.8 循環伏安法量測 42
3.2.2.9 交流阻抗法量測 42
3.3 結果與討論 42
3.3.1 DNA 分子自組裝於金電極表面的覆蓋率 42
3.3.2 以電泳分析以及 XPS 檢測 Ni-DNA 之形成 46
3.3.3 DNA 與 Ni-DNA 之間電子特性的差異 50
3.3.4 電化學分析 51
3.3.4.1 以循環伏安法分析 DNA 與 Ni-DNA 之電化學特性 51
3.3.4.1.1 不同電解質溶液系統對 DNA 分子電化學特性的影響 51
3.3.4.1.2 DNA 與 Ni-DNA 之電化學特性 55
3.3.4.1.3 Ni-DNA 的電導機制 55
3.3.4.2 以交流阻抗法分析 DNA 與 Ni-DNA 之電性 58
3.3.4.2.1 DNA 與 Ni-DNA 之阻抗圖譜 58
3.3.4.2.2 等效電路模擬 61
3.3.4.2.3 鹼基對堆疊對 Ni-DNA 電性的影響 63
3.3.5 Ni-DNA 於生物感測器上的應用 66
3.3.5.1 DNA 序列中鹼基對錯誤配對之檢測 67
3.4 結論 70
第四章 DNA 分子元件製作與電性量測 72
4.1 前言 72
4.2 實驗 72
4.2.1 實驗藥品、溶液配製與設備 72
4.2.2 實驗操作步驟 74
4.2.2.1 電極製作 75
4.2.2.2 DNA 溶液中多餘金屬離子及鹽類的透析 75
4.2.2.3 DNA 分子的electrostatic trapping 76
4.2.2.4 電性量測 77
4.2.2.5 DNA 分子影像分析 77
4.2.2.6 銀離子交換法 77
4.3 結果與討論 78
4.3.1 Ni-DNA 與 ��-DNA 之形貌分析 78
4.3.2 Electrostatic trapping 81
4.3.3 DNA 分子元件之電性量測 84
4.3.3.1 鹽類殘留對電性的影響 85
4.3.3.2 ��-DNA 與 Ni-DNA 之電性量測 86
4.3.3.3 Ni-DNA 分子元件之負微分電阻特性 87
4.3.3.4 不同掃描速率對負微分電阻的影響 89
4.4 結論 90
第五章 總結 92
參考文獻 93

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