毛細管電泳質譜嵌合式/一體式雙槽介面研究暨應用

The Study and Application of an Assembled/Integrated Double Junction Interface for Capillary Electrophoresis Electrospray Ionization-Mass Spectrometry

彭奎翰(Kuei-Han Peng)

指導教授 ： 何國榮

國立臺灣大學/理學院/化學研究所/碩士(2012年)

https://doi.org/10.6342/NTU.2012.02130

摘要

本論文利用實驗室已開發之聚二甲基矽氧烷(Polydimethylsiloxane, PDMS一體式雙槽介面銜接微胞電層析質譜(MEKC-ESI/MS)分析九種磺胺類藥物以解決微胞對分析物訊號的抑制。一體式雙槽介面為在PDMS基材上灌鑄雙槽及連接雙槽的微通道，分離毛細管及電灑噴頭分別銜接於微通道的兩端，微胞電層析於分離管內完成分析後，微通道內藉由PDMS材質本身提供的低電滲流，使分離管出來的微胞(Ammonium dodecyl sulfate, ADS)因負淌度大於微通道的電滲流而不會被帶往質譜端。一體式雙槽介面相較於實驗室曾發表的液體接合式-低流速鞘流介面容易組裝操作，且應用於相同分析系統，可提供較佳的訊號靈敏度。此外雙槽間之距離僅1公分，可保留原本毛細管電泳系統之分離結果。

為了擴充此介面在不同電泳系統的應用，本論文由一體式雙槽介面衍生出嵌合式一體雙槽介面，將其PDMS微通道改為一嵌合式的毛細管，藉著替換不同材質毛細管而可變換電滲流以適應不同的系統需要。論文中分別以玻璃毛細管及聚合物PEEK (polyether ether ketone)材質作嵌合毛細管：以玻璃毛細管作嵌合毛細管的實驗裡，使用添加有機相的策略以降低電滲流使微胞回退，應用於微胞電層析系統；以聚合物PEEK材質毛細管作嵌合毛細管的實驗中，應用於磷酸系統分析核苷酸，在pH 10.0的條件下，利用其電滲流介於磷酸根及核苷酸回退速度的特性，達成在嵌合毛細管中使抑制性的磷酸根離子回退，並將核苷酸帶往質譜端偵測。

關鍵字

一體式雙槽介面 ； 微胞電層析質譜 ； 聚二甲基矽氧烷 ； 毛細管電泳質譜 ； PEEK毛細管

並列摘要

In this thesis, using the PDMS-based integrated double junction interface which was developed by latest work of our lab alleviate the ion suppression caused by micelles for Micellar Electrokinetic Chromotagraphy-Electrospray Ionization-Mass Spectrometry (MEKC-ESI/MS) to analyze nine sulfonamides.The integrated double junction interface is consisted of two junctions and a connecting microchannel grouted by PDMS. The separation capillary column and sprayer are connected to each side of the microchannel. After separated by MEKC in separation column, micelles are moving backward in PDMS microchannel which has the lower rate of electroosmotic flow than micelles. Therefore, that keeps micelles moving away from mass source to alleviate the ion suppression by using PDMS microchannel. In addition, the integrated double junction interface can be fabricated by easier approach than lowflow-liquid junction interface published by our lab in the past and provide better sensitivity in the same buffer system. In the other hand, the original separation efficiency can be reserved because there is only 1 cm distance between junction to junction.

In order to enrich the application on different buffer systems of this interface, using an assembled column instead the PDMS microchannel, which is called the assembled integrated double junction , derivated from the integrated double junction. By using different materials of columns can reach different EOF which is needed in different buffer systems. In this thesis, bared silica column and PEEK column are used as the assembled column. In the work of silica, adding organic solvent is employed as the way to lower down the EOF, leading to micelles moving backward,that is applicated on MEKC system to analysis the sulfonamides. And in the work of PEEK, to lower down the EOF by the naturality of the material. It is successful to applicate on the phosphate buffer system to analysis the oligonucleotides in pH 10 buffer condition, because the phosphate anion moves backward in PEEK column as the assembled column, whereas oligonucleotides are carried to the mass detector by EOF of PEEK.

並列關鍵字

the integrated double junction interface ； MEKC-ESI/MS ； PDMS ； capillary electrophoresis mass spectrometry ； PEEK capillary column

參考文獻

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