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Student Number 952403007
Author Yuan-chang Su(蘇源昌)
Author's Email Address 952403007@cc.ncu.edu.tw
Statistics This thesis had been viewed 563 times. Download 234 times.
Department Chemistry
Year 2010
Semester 2
Degree Ph.D.
Type of Document Doctoral Dissertation
Language zh-TW.Big5 Chinese
Title Development and Applications of Automated Gas Chromatography-Mass Spectrometry for the Analysis of Volatile Organic Compounds
Date of Defense 2011-07-07
Page Count 237
Keyword
  • GC-MS
  • volatile organic compounds
  • Abstract The objective of this research is to develop an automated gas chromatographic mass spectrometry (GC-MS) system for monitoring volatile organic compounds (VOCs). The content divides into two parts. The first part describes the technical improvement of the automated GC-MS system. The second part is to apply the developed system to measure VOCs in the field.
    There are three subjects comprised in the first part of technical improvements. (1) The split mechanism of injection was introduced into chromatographic system. The mechanism reduces two main factors of extra column effect, Vtub2 and Vinj2, to enhance resolution of chromatogram resulted in improving processing data efficiency and data quality. (2)Two-dimensional chromatographic (heart-cutting) technique was applied to GC-MS system. We have developed two operational modes naming “hold-up method” and “backflush & trap method”. The parameters and resolutions of the two modes were tuned and compared with each other. The optimized condition of the system was capable to measure the full range of VOCs from C3 to C12. (3) In this research, we have investigated the sorption/desorption properties and applicability of MCM-48 as a sorbent for on-line gas chromatographic analysis of ambient VOCs. Two trapping temperatures of 30°C versus -20°C were tested by trapping a full range of VOCs from C2 to C12. The required desorption temperatures of MCM-48 (100-180°C) were much lower than carbon sorbents(>200°C). As a result, the large pores of MCM-48 with low memory effect can desorb VOCs more efficient.
    In field campaigns, the air qualities of three industrial parks (Kuangin of Taoyuan County, Dafa of Gaoxiong County, and Sixth Naphtha Cracking of Yunlin County) were investigated. The data of in-situ monitoring site acquired by GC-MS were compared with analysis of off-line sampling and commercial mass spectrometry in order to examine their reliability and efficacy. The analysis of off-line sampling as well as GC-MS has the capability of establishing the list of VOC in industrial park and data measured by commercial mass spectrometry and GC-MS are in agreement on trend of VOC. In the end, the data provided by in-situ GC-MS system and Wind Model can verify and compromise each other. The results have confirmed the utility and applicability of GC-MS in a standard operation procedure of monitoring VOC.
    Table of Content 目錄
    第一章 緒論.................................................................................................1
    1-1 VOC簡介...................................................................................................6
    1-2 人工採樣方法.........................................................................................10
    1-3 自動即時監測技術.................................................................................15
    1-4 前濃縮系統概念.....................................................................................21
    1-5 層析管柱.................................................................................................25
    第二章 進樣與分流機制........................................................................29
    2-1 額外管柱增寬效應.................................................................................32
    2-2 捕捉管口徑的影響.................................................................................34
    2-3 分流機制的影響.....................................................................................40
    2-3.1 注射帶..........................................................................................40
    2-3.2 分流比例最佳化..........................................................................45
    2-4 小結……………….................................................................................57
    第三章 二維氣相層析質譜儀之研究.................................................59
    3-1 丁氏切換裝置與應用.............................................................................63
    3-2 實驗系統架構.........................................................................................75
    3-2.1 前濃縮系統..................................................................................75
    3-2.2 層析系統......................................................................................76
    3-3 氣流控制模式.........................................................................................79
    3-3.1 滯留法..........................................................................................80
    3-3.2 逆吹法..........................................................................................84
    3-4 系統線性與再現性.................................................................................90
    3-5 層析峰寬、對稱性、解析度..................................................................93
    3-6 小結……………….................................................................................98
    第四章 中孔徑吸附劑之應用研究......................................................99
    4-1 吸附材料特性.......................................................................................102
    4-2 前濃縮系統與層析系統.......................................................................106
    4-2.1 冷凍前濃縮系統........................................................................107
    4-2.2 冷凍捕捉裝置與捕捉管............................................................109
    4-2.3 層析系統....................................................................................112
    4-3 結果與討論…………….......................................................................115
    4-3.1 低碳數物種捕捉效率................................................................115
    4-3.2 高碳數物種捕捉效率................................................................118
    4-3.3 線性與再現性………................................................................120
    4-3.4 脫附溫度曲線………................................................................126
    4-3.4 記憶效應……………................................................................137
    4-4 小結.......................................................................................................139
    第五章 自動監測層析質譜儀之應用...............................................141
    5-1 工作方法...............................................................................................144
    5-1.1 環保署即時監測站....................................................................144
    5-1.2 層析質譜儀即時監測系統........................................................147
    5-1.3 離子分子反應質譜儀................................................................153
    5-1.4 質子轉移質譜儀儀....................................................................156
    5-1.5 人工採樣方法............................................................................160
    5-2 人工採樣法與GC-MS比對..................................................................165
    5-3 快速質譜儀與GC-MS比對..................................................................180
    5-4 風場模式與GC-MS比對......................................................................202
    5-5 小結.......................................................................................................211
    第六章 總結與未來展望......................................................................215
    參考文獻 ..................................................................................................219
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    第二章
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    第三章
    1.Helmig, D., Air analysis by gas chromatography. Journal of Chromatography A 1999, 843, (1-2), 129-146.
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    第四章
    1.Dewulf, J.; Van Langenhove, H., Anthropogenic volatile organic compounds in ambient air and natural waters: a review on recent developments of analytical methodology, performance and interpretation of field measurements. Journal of Chromatography A 1999, 843, (1-2), 163-177.
    2.Helmig, D., Air analysis by gas chromatography. Journal of Chromatography A 1999, 843, (1-2), 129-146.
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    第五章
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    3.Lin, T.-Y.; Sree, U.; Tseng, S.-H.; Chiu, K. H.; Wu, C.-H.; Lo, J.-G., Volatile organic compound concentrations in ambient air of Kaohsiung petroleum refinery in Taiwan. Atmospheric Environment 2004, 38, (25), 4111-4122.
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    5.Jia, C.; Batterman, S.; Godwin, C., VOCs in industrial, urban and suburban neighborhoods, Part 1: Indoor and outdoor concentrations, variation, and risk drivers. Atmospheric Environment 2008, 42, (9), 2083-2100.
    6.Jia, C.; Batterman, S.; Godwin, C., VOCs in industrial, urban and suburban neighborhoods--Part 2: Factors affecting indoor and outdoor concentrations. Atmospheric Environment 2008, 42, (9), 2101-2116.
    7.Kim, K.-H.; Hong, Y.-J.; Pal, R.; Jeon, E.-C.; Koo, Y.-S.; Sunwoo, Y., Investigation of carbonyl compounds in air from various industrial emission sources. Chemosphere 2008, 70, (5), 807-820.
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    11.Mudliar, S.; Giri, B.; Padoley, K.; Satpute, D.; Dixit, R.; Bhatt, P.; Pandey, R.; Juwarkar, A.; Vaidya, A., Bioreactors for treatment of VOCs and odours - A review. Journal of Environmental Management 2007, 91, (5), 1039-1054.
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    13.Wang, J.-L.; Chen, S.-W.; Chew, C., Automated gas chromatography with cryogenic/sorbent trap for the measurement of volatile organic compounds in the atmosphere. Journal of Chromatography A 1999, 863, (2), 183-193.
    14.Wang, J.-L.; Chen, W.-L.; Lin, Y.-H.; Tsai, C.-H., Cryogen free automated gas chromatography for the measurement of ambient volatile organic compounds. Journal of Chromatography A 2000, 896, (1-2), 31-39.
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    22.Jimenez, J. L.; Farmer, D. K., Real-time Atmospheric Chemistry Field Instrumentation Analytical Chemistry 82, (19), 7879-7884.
    23.Wang, J.-L.; Chew, C.; Chen, S.-W.; Kuo, S.-R., Concentration Variability of Anthropogenic Halocarbons and Applications as Internal Reference in Volatile Organic Compound Measurements. Environmental Science & Technology 2000, 34, (11), 2243-2248.
    24.Wang, J.-L.; Lin, W.-C.; Chen, T.-Y., Using atmospheric CCl4 as an internal reference in gas standard preparation. Atmospheric Environment 2000, 34, (25), 4393-4398.
    25.Karbiwnyk, C. M.; Mills, C. S.; Helmig, D.; Birks, J. W., Use of Chlorofluorocarbons as Internal Standards for the Measurement of Atmospheric Non-Methane Volatile Organic Compounds Sampled onto Solid Adsorbent Cartridges. Environmental Science & Technology 2003, 37, (5), 1002-1007.
    26.Chang, C.-C.; Lo, G.-G.; Tsai, C.-H.; Wang, J.-L., Concentration Variability of Halocarbons over an Electronics Industrial Park and Its Implication in Compliance with the Montreal Protocol. Environmental Science & Technology 2001, 35, (16), 3273-3279.
    27.Wanke, T.; Vehlow, J. g., IMR-MS on-line measurements in the exhaust gas of a municipal solid waste incineration pilot plant (Tamara). Chemosphere 1997, 34, (2), 345-355.
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    29.Chang, C.-C.; Lo, S.-J.; Lo, J.-G.; Wang, J.-L., Analysis of methyl tert-butyl ether in the atmosphere and implications as an exclusive indicator of automobile exhaust. Atmospheric Environment 2003, 37, (34), 4747-4755.
    30.郭姝涵; 王國英, 高解析度空氣污染物擴散模擬模式的發展. 中央大學大氣物理研究所 民國九十九年六月.
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  • Jia-Lin Wang(王家麟)
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    Date of Submission 2011-07-19

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