真空加熱矽奈米結構晶片對於提升質譜檢測靈敏度與離子化機制探討與應用

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姓名

林園景(Lin Yuan Jing) 查詢紙本館藏

畢業系所

機械工程學系

論文名稱

真空加熱矽奈米結構晶片對於提升質譜檢測靈敏度與離子化機制探討與應用

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摘要(中)

質譜分析是檢測蛋白質與胜肽樣本的重要工具，應用在許多生物醫學、細胞代謝檢測分析上，如今質譜檢測快速發展，檢測技術朝向以無機質的固態材料為基材，稱之為表面輔助雷射脫附游離法（Surface-assisted Laser Desorption Ionization , SALDI），而本研究使用金屬輔助蝕刻製作出奈米層狀矽結構 (nanostructured silicon , nSi)，此結構具有高的表面積可吸收紫外光，檢測分析上具有高靈敏度且不受基質干擾。
本研究將奈米矽晶片放置於不同環境下，觀察質譜訊號與接觸角的變化，發現放置於真空與氮氣環境下能保持質譜性能與維持表面疏水性。另外提出利用真空加熱奈米矽晶片的處理方式，不僅能提升晶片表面疏水性，還可提高質譜晶片檢測的靈敏度，檢測濃度10-6M的des-Arg9 Breakinin樣本可提升六倍的質譜訊號，且樣本檢測極限達到從10-7M 提升至10-10M，並且可消除低質量區域景雜訊的干擾，有利於小分子量的樣本分析。
從真空加熱實驗中探討DIOS的機制，由螢光吸附結果得知，真空加熱後的晶片樣本吸附方式較為不同，推理出加熱後的模型，說明表面分析物經由吸收更多熱能達到脫附。另外發現表面經由空氣生成的氧化物對於質譜訊號並不會造成負面影響，且推測與目前學者所提出的離子源Si-OH為同一物質，並利用二次沉積方式將金粒子覆蓋於表面，輔助證明表面離子源。

摘要(英)

Mass spectrometry (MS) is an important instrument for the detection of protein and peptide samples which have been widely used in biomedical and cytology fields. Recent trends of mass spectrometry focus on developing solid inorganic materials called Surface-assisted Laser Desorption Ionization, SALDI. In this study we use metal-assisted chemical etching process to fabricate nanostructured silicon. This nanostructure has high surface area which can absorb UV light during MS analysis. The MS analysis exhibit high sensitivity and without matrix interference performance.
In this study, we investigate nanostructured silicon chip storing desorption/ionization efficiency in various environments. We found MS performance and surface hydrophobic are well preserved under vacuum and nitrogen conditions. We also propose nanostructured silicon chips storage using a vacuum heat treatment. The hydrophobicity of the wafer surface can not only enhanced, but the MS detection sensitivity can also improve. We detect 10-6 M des-Arg9 bradykinin can enhance six times and detection limit enhanced to10-7 M to 10-10 M.

關鍵字(中)

★ 多孔矽
★ 質譜分析
★ 表面輔助雷射脫附游離法

關鍵字(英)

★ porous silicon
★ mass spectrometry
★ SALDI

論文目次

摘要 ................................I
Abstract................................II
目錄 ................................IV
圖目錄..................................VII
第一章簡介...............................1
1-1質譜檢測的發展.........................1
1-2 多孔矽晶片保存.......................11
1-3研究目的..............................17
第二章材料與方法.........................19
2-1實驗材料與藥品.........................19
2-2實驗設備與分析儀器.....................20
2-3實驗流程..............................21
2-3奈米矽晶片製作........................22
2-3-1晶片前處理..........................22
2-3-2沉積金薄膜..........................22
2-3-3金屬輔助蝕刻........................23
2-4 BOE去除氧化層........................23
2-5真空加熱..............................24
2-6質譜分析.............................24
2-7接觸角量測............................28
2-8螢光吸附測試..........................28
2-9二次沉積..............................29
2-10 COOH負電性官能基表面改質法............30
第三章結果與討論..........................32
3-1奈米矽結構..............................32
3-2環境對晶片性能的影響.....................34
空氣環境...................................34
甲醇環境...................................36
真空環境...................................38
氮氣環境....................................40
3-3真空加熱對nSi晶片的影響...................44
3-4改變晶片表面特性.........................48
3-5 真空加熱對於小分子雜訊與.................58
3-6檢測靈敏度之探討..........................60
3-7長時間保存................................62
3-8二次沉積晶片與表面改質.....................65
3-8-1金粒子驗證..............................65
3-8-2質譜分析................................67
3-8-3 離子源探討..............................69
第四章結論與未來展望..........................71
4-1結論......................................71
4-2未來展望..................................73
第五章參考文獻...............................74
附錄.........................................79

參考文獻

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指導教授

曹嘉文

審核日期

2015-7-7

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