자료유형 | 학위논문 |
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서명/저자사항 | Development of Functionalized Paper-Based Sample Collection and Direct Mass Spectrometry Analysis Platforms. |
개인저자 | Damon, Deidre Erin. |
단체저자명 | The Ohio State University. Chemistry. |
발행사항 | [S.l.]: The Ohio State University., 2019. |
발행사항 | Ann Arbor: ProQuest Dissertations & Theses, 2019. |
형태사항 | 188 p. |
기본자료 저록 | Dissertations Abstracts International 81-06B. Dissertation Abstract International |
ISBN | 9781687972125 |
학위논문주기 | Thesis (Ph.D.)--The Ohio State University, 2019. |
일반주기 |
Source: Dissertations Abstracts International, Volume: 81-06, Section: B.
Advisor: Badu-Tawiah, Abraham. |
이용제한사항 | This item must not be sold to any third party vendors. |
요약 | The goal of this dissertation is to develop a paper-based mass spectrometry (MS) ionization method for detection of small molecules from biological fluids and water samples. In biofluids, highly sensitive analytical methods are required to monitor small biologically active molecules during treatment. When analyzing both biofluids and industrial water samples, rapid and inexpensive detection platforms streamline screening for harmful concentrations of chemicals. Paper spray ionization shortens analysis time to less than one minute.Current analytical detection methods for these molecules include gas chromatography (GC)-MS, which is useful for creating databases for small molecules. However, GC-MS often requires extensive sample preparation and analyte derivatization prior to analysis. Liquid chromatography (LC)-MS offers better sensitivity without the need for derivatization. However, LC-MS is also limited by additional sample preparation/handling procedures. In particular, matrix components must be removed prior to any chromatographic work, which can be time consuming. For these reasons, immunoassay screening is still the most commonly used detection method for these small molecules despite their well-recognized limitations with regards to sensitivity and selectivity. Alternatively, paper spray (PS) ionization MS is capable of direct analysis of small biological sample volumes. However, PS often suffers from low sensitivity due to inefficient extraction.The second chapter in this document utilizes treated hydrophobic paper substrates prepared by a gas-phase silanization reaction. Hydrophobic PS utilizes online liquid/liquid extraction from a drop of biological fluid without drying steps or sample pretreatment, which is applicable in point-of-care analyses. Preliminary experiments demonstrated high sensitivity in the analysis of drugs cocaine, benzoylecgonine, methamphetamine, and amphetamine in 4 關L of raw blood, serum, and urine. When the sample is dried, a 3-dimensional dried spheroid is formed, as opposed to a dried blood spot. This spheroid decreases interaction between the bulk of the blood sample and ambient air, decreasing oxidative stress, increasing the lifetime of the analyte in the sample. Experiments show that labile organic compounds diazepam and cocaine have increased stability up to 28 days, where sample signal decreases by 90% within a day when stored in dried blood spots.The third chapter discusses the use of wax printing on paper. Wax printing creates microfluidic channels in which the designer can control solvent flow. Through this solvent control, spray time was increased from 1.5 minutes to 10 minutes. Additionally, because the solvent acts as the charge carrier, manipulation of the electric field decreased the required voltage applied to the paper triangle from 3-5 kV to 0.5-1 kV.The fourth chapter outlines the detection of low concentration corrosion inhibitor Duomeen O and molluscicide metaldehyde in industrial and environmental water samples. On-site analysis of Duomeen O would facilitate the maintaining of appropriate levels to prevent corrosion in water tube boiler plants. Because metaldehyde is readily soluble in water, runoff during periods of heavy rainfall ultimately introduces metaldehyde into drinking water. Paper spray ionization has been demonstrated as a viable technique for rapid screening and quantification of these molecules without sample preconcentration with detection limits below the threshold set by the World Health Organization. |
일반주제명 | Chemistry. Health sciences. Biochemistry. |
언어 | 영어 |
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