跳到主要內容

臺灣博碩士論文加值系統

(34.236.36.94) 您好!臺灣時間:2021/07/24 22:58
字體大小: 字級放大   字級縮小   預設字形  
回查詢結果 :::

詳目顯示

我願授權國圖
: 
twitterline
研究生:曾偉志
研究生(外文):Wei-chih Tzeng
論文名稱:醛酮類有機物檢測與環境因子相關性之研究
論文名稱(外文):A Study on the Correlation between Environmental Factors and Analyses of Aldehydes and Ketones
指導教授:林達昌
指導教授(外文):Ta-Chang Lin
學位類別:碩士
校院名稱:國立成功大學
系所名稱:環境工程學系碩博士班
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2008
畢業學年度:96
語文別:中文
論文頁數:94
中文關鍵詞:2 4-DNPH環境條件固相吸附管醛酮HPLC
外文關鍵詞:ketonescartridge2 4-DNPHaldehydesenvironmental factors
相關次數:
  • 被引用被引用:3
  • 點閱點閱:238
  • 評分評分:
  • 下載下載:0
  • 收藏至我的研究室書目清單書目收藏:0
空氣中醛酮化合物的汙染對環境影響逐漸增加,而同時台灣地區近年對於各醛酮污染源的排放限制其法規和檢測機制仍未臻完善,尤其煙道的固定污染源中酮類化合物之排放,其檢測環境條件變數較一般大氣複雜,現今常用於醛酮化合物的檢測法以2,4-DNPH衍生法為主,以HPLC層析後配合UV 偵測器對醛酮衍生物進行定性定量分析。並選擇常見於工廠使用的有機溶劑丙酮、2-丁酮和甲基異丁酮,配以有較完善採樣法的甲醛和乙醛,進行模擬煙道環境下溫度、含水率和SOX/NOX 濃度各條件改變,對濕式吸收瓶法與固相吸附管法於這五種醛酮類採樣上的影響,並提供一煙道醛酮採樣方法的建議。
研究結果顯示,環境條件對於不同採樣法的醛酮回收率各有不同影響,醛酮回收率主要與溫度(80 ℃∼200 ℃)和SOX/NOX 濃度條件呈中高度負相關性,與含水率條件(0∼19 vol%)為低度負相關,但環境含水率卻令與溫度和SOX/NOX 濃度條件有不同的交互影響作用,含水率的增加會減少溫度與醛酮回收率的負干擾,卻提高SOX/NOX 濃度條件對於醛酮回收率的負干擾。經過實驗評估得知濕式吸收瓶採樣法比吸附管採樣法不易受環境變數干擾,且其醛酮回收率較也相對穩定,並當吸收瓶採樣法中的吸收液過氯酸濃度調整為1 mmol/L 時,甲醛回收率可達105 %、乙醛回收率為96 %、丙酮回收率為90 %、2-丁酮回收率達100 %、甲基異丁酮回收率達75 %。
The pollutant of aldehydes and ketones in the atmosphere has been increasing gradually. In Taiwan, regulations and analytic method for aldehydes and ketones are not yet perfect, especially for ketones in stationary sources. The environment factors in stationary sources are more complicated than in ambient air. After derivatizing the aldehydes and ketones with 2,4-dinitrophenyl- hydrazine (DNPH), the derivatives are then analyzed by
HPLC with UV detection.
In the study, we chose acetone, 2-butanone, and methyl isobutyl ketone that are common organic solvent in factories. In addition, we also studied formaldehyde and acetaldehyde in sampling under various temperature conditions, moisture loading factors, and concentration of SOX and NOX. Both impinger and cartridge methods were used to sample the five carbonyl compounds. From the final correlation found between environmental factors and analyses of aldehydes and ketones, we are able to provide
recommendations for improving sampling and analyses of aldehydes and ketones.
The result shows that environment variables have different effects on the sampling and analysis of the five carbonyls. There is large negative correlation between temperature factors (80 °C~200 °C) and the recovery. A
small negative correlation was also found between moisture loading factors (0~14 vol %) and the recovery. Otherwise, when the moisture loading increased, interference by temperature became smaller, while the interference by SOX/NOX grew.
This study found out that between the cartridge method and the impinger methods, the former is more susceptible to changes in environmental conditions. Therefore the impinger method, being more robust and reliable, is recommended. The best recovery in carbonyls, obtained when the concentration of HClO4 in the DNPH reagent was 1 mM, were respectively 105 %, 96 %, 90 %, 100 %, and 75% for formaldehyde, acetaldehyde, acetone, 2-butanone, and methyl isobutyl ketone.
第一章 前言……………………………………………………………1
1-1 研究動機……………………………………………………………1
1-2 研究目的……………………………………………………………2
第二章 文獻回顧………………………………………………………3
2-1 國內外醛、酮類有機物檢測技術…………………………………3
2-1.1 國外醛、酮類化合物之檢測方法………………………………5
2-1.2 國內醛酮檢測方法應用概述……………………………………8
2-2 實驗室醛、酮類有機物分析技術研究…………………………11
2-3 醛酮檢測法的干擾影響因素……………………………………18
第三章 實驗方法與步驟………………………………………………21
3-1 採樣設計與程序…………………………………………………24
3-1.1 藥品及試劑……………………………………………………24
3-1.2 系統環境條件控制……………………………………………26
3-1.3 採樣流程………………………………………………………27
3-1.4 樣品前處理……………………………………………………31
3-2 儀器與分析條件…………………………………………………32
3-2.1 儀器設備………………………………………………………32
3-2.2 HPLC分析程序…………………………………………………32
3-2.3 層析梯度設定…………………………………………………33
3-3 數據處理…………………………………………………………39
3-3.1 儀器數據分析…………………………………………………39
3-3.2 實驗數據統計分析……………………………………………39
第四章 實驗之品質保證與控制………………………………………41
4-1 檢量線品保品管…………………………………………………41
4-1.1 檢量線製備……………………………………………………41
4-1.2 儀器偵測極限及儀器精確度準確度…………………………41
4-1.3 檢量線之確認…………………………………………………42
4-1.4 滯留時間測試…………………………………………………42
4-1.5 方法準確度和精密度建立……………………………………42
4-2 空白分析…………………………………………………………43
4-3 吸附管萃取效率…………………………………………………43
4-4 貫穿測試…………………………………………………………44
4-5 重複分析…………………………………………………………44
4-6 吸附管最佳流量測試……………………………………………44
4-7 樣品存放時間分析………………………………………………46
4-8 液針體積定量……………………………………………………47
第五章 實驗結果與討論………………………………………………49
5-1 吸收液採樣法與五種醛酮的回收率試驗………………………49
5-1.1 吸收液回收率試驗……………………………………………51
5-1.2 吸收液採樣法與溫度變數的相關性…………………………56
5-1.3 吸收液採樣法與含水率變數的相關性………………………58
5-1.4 吸收液採樣法與SOX/NOX濃度變數的相關性…………………60
5-1.5 環境變數對於吸收液採樣法的影響…………………………62
5-1.6 過氯酸濃度與醛酮衍生反應的影響…………………………63
5-2 吸附管採樣法與五種醛酮類的回收率試驗……………………65
5-2.1 吸附管採樣法與溫度變數的相關性…………………………69
5-2.2 吸附管採樣法與含水率變數的相關性………………………70
5-2.3 吸附管採樣法與NOX/SOX濃度變數的相關性…………………72
5-2.4 環境變數對於吸附管採樣法的影響…………………………74
第六章 結論與建議……………………………………………………75
6-1 結論………………………………………………………………75
6-2 建議………………………………………………………………77
參考文獻………………………………………………………………79
附錄A 方法準確度精密度和偵測極限………………………………86
附錄B 檢量線公式(梯度程式A)……………………………………89
檢量線公式(梯度程式B)……………………………………90
附錄C 儀器偵測極限…………………………………………………91
附錄D 儀器精密度與準確度…………………………………………92
附錄E 十七種醛酮滯留時間…………………………………………93
A. Levart, M. Veber, “Determination of aldehydes and ketones in air samplings using cryotrapping sampling”, Chemosphere.44:701-708., 2001
APHA Method 122, “Determination of C1-C5 aldehydes in ambient air and source emissions as 2,4-dinitrophenylhydrazones by HPLC.”
Beasley R.K., Hoffmann C.E., Rueppel M.L. and Worley J.W., “Sampling of formaldehyde in air with coated solid sorbent and determination by high performance liquid chromatography” , Anal.Chem. 52:1110., 1980
CARB, SOP No. 104., “Determination of aldehyde and ketone compounds in automotive source samples by high performance liquid chromatography.”
CARB, SOP No. 022., ”Standard operating procedure for the determination of carbonyl compounds in ambient air.”
Cohen I. R. and Altshuller A. P., “A new spectrophotometric method for the determination of acrolein combustion gases and in the atmosphere” , Anal. Chem., 33:726-733., 1961
Coutrim MX, Nakamura LA, Collins CH., “Quantification of 2,4-dinitrophenyl-hydrazones of low molecular mass aldehydes and ketones using HPLC”, Chromatographia.37:185–90., 1993
C. C. Hsieh, J. H. Tsai, “VOC concentration characteristics in southern taiwan” , Chemosphere. 50:545-556., 2003
De Andrade JB, Pinheiro HLC, Andrade MV., “Determination of formaldehyde and acetaldehyde associated atmospheric aerosols by HPLC.” Intern J Environ Anal Chem. 52:49–56., 1993
Fung K, Grosjean D., “Determination of nanogram amounts of carbonyls as 2,4-dinitrophenylhidrazones by high-performance liquid chromatography”, Anal Chem. 53:166–71., 1981
Gioacchini AM, Roda A, Galletti GC, Bocchini P, Manetta AC, Baraldini M., “High-performance liquid chromatography-electrospray mass spectrometric analysis of phenolic acids and aldehydes”, J chromatogr. A 1996:730:31–37., 1996
Goldschmidt BM., “Role of aldehydes in carcinogenesis.” J Environ Sci Health, 2:231–49., 1984
Groemping A. H. J. and Cammann K., “Development and comparison of different fluorimetric HPLC-methods with standard methods for the determination of formaldehyde in the atmosphere”, Chromatographia, 35:142-148., 1993
Grosjean D.,“Formaldehyde and other carbonyls in Los Angeles ambient air”, Environ.Sci. Technol., 16:254-262., 1982
Grosjean D. and Fung K., “Collection efficiencies of cartridges and microimpingers for sampling of aldehydes and ketones as 2,4-dinitrophenylhydrazones”, Anal. Chem., 54:1221-1224., 1982
H.L.C. Pinheiro, M.V. de Andrade, P.A. de Paula Pereira, J.B. de Andrade., “Spectrofluorimetric determination of formaldehyde in air after collection onto silica cartridges coated with Fluoral P” ,Microchemical Journal. 78:15-20., 2004
Ho S. S. H, Yu J.Z., “Determination of airborne carbonyls: comparison of a thermal desorption/gc method with the standard dnph/hplc method”, Environ. Sci. Technol. 38:862-870., 2004
I. D. Williams, D. M. Revitt, R. S. Hamilton., “A comparison of carbonyls compound concentration at urban roadside and indoor sites” , The Science of the total Environment. 189/190:475-483., 1996
Karst. U. et al., “Interferences of nitrogen dioxide in the determination of aldehydes and ketones by sampling on 2,4-dinitrophenylhydrazine-coated solid sorbent”, Fresenius J. Anal. Chem., 345:48-52., 1993
Magin J. Chromatogr D. F., “Preparation and gas chromatographic characterization of benzyloximes and p-nitrobenzyloximes of short-chain(C1-C7) carbonyls”, Journal of Chromatography, 178:219-227., 1979
Magin J. D. F., “Gas chromatography of simple monocarbonyls in cigarette whole smoke as the benzyloxime derivatives”, Journal of Chromatography, 202:255-261., 1980
Nishikawa H. et al., ”Determination of micro amount of acrolein in air by gas chromatography, Journal of Chromatography”, 370:327-333., 1986
Nishikawa, H. and Sakai, T., “Derivatization and Chromatographic Determination of Aldehydes in Gaseous And Air Samples”, Journal of Chromatography”, A 710:159-165., 1995
Nondek L. et al., “Determination of carbonyl compounds in air by HPLC using on-line analyzed microcartridges, fluorescence and chemilumines detection”, Chromatographia, 32:33-39., 1991
Olson K. L. and Swarin S. J., “Determination of aldehydes and ketones by derivatization and liquid chromatography-mass spectrometry” ,J. Chromatogr., 333:337-347., 1985
Papa LJ, Turner LP., “Chromatographic determination
of carbonyl compounds as their 2,4-dinitrophenylhydrazones I. Gas chromatography”, J Chromatogr Sci. 10:744–7., 1972
Peter J. O’Brien, Arno G. Siraki, and Nandita Shangari., “Aldehyde sources, metabolism, molecular toxicity mechanisms, and possible effects on human health”, Critical Reviews in Toxicology (2005) 35: 609–662., 2005
Peters R, Hellenbrand J, Mengerink Y, Van der Wal SJ., “On-line determination of carboxylic acids, aldehydes and ketones by high-performance liquid chromatography-diode array detection-atmospheric chemical ionization mass spectrometry after derivatization with 2-nitrophenylhydrazine”, J chromatogr. A 2004: 1031:30-50., 2004
R. Pestman, A van Duijne, J.A.Z. Pieterse, V. Ponec., “The formation of ketones and aldehydes from carboxylic acids, structure-activity relationship for two competitive reactions”, J Molecular Catalysis A:CHEMICAL 103(1995)175-180., 1995
Sakuragawa A, Yoneno T, Inoue K, Okutani T., “Trace analysis of carbonyl compounds by liquid chromatography-mass spectrometry after collection as 2,4-dinitrophenylhydrazine derivatives”. J chromatogr. A 1999:844:403-408., 1999
Selim S., “Separation and quantitative determination of traces of carbonyl compounds as their 2,4-dinitrophenylhdrazones by high-pressure liquid chromatography”, Journal of Chromatography, 136:271-277., 1977
Swarin S. J. and Lipari F., “Deternation of formaldehyde and other aldehydes by high performance liquid chromatography with fluorescence detection”, Journal of Liquid Chromatography, 6:425-444., 1983
Tanner R.L. and Meng Z., “Seasonal variations in ambient atmospheric levels of formaldehyde and acetaldehyde “, Environ. Sci. Technol. 18:723-726., 1984
USEPA, Method IP-6., “Determination of formaldehyde and other aldehydes in indoor air”
USEPA, Method TO-11A. “Aldehydes/ketones from DNPH adsorbents by HPLC”
USEPA, Method TO-15A .”Volatile organic compounds (polar/non-polar) from canisters by GC/MS”
USEPA, Method TO-5. “Method for the determination of aldehydes and ketones in ambient air using high performance liquid chromatography (HPLC)”
USEPA, Method TO-11A: “Determination of Formaldehyde in Ambient Air Using Adsorbent Cartridge Followed by High Performance Liquid Chromatography (HPLC)”.
USEPA, Method TO-5:, “Determination of Aldehydes and Ketones in Ambient Air Using High Performance Liquid Chromatography (HPLC)”.
USEPA, Method 0011., “Sampling for selected aldehyde and ketone emissions from stationary sources”.
USEPA, Method 316., “Sampling and analysis for formaldehyde emissions from stationary sources in the mineral wool and wool fiberglass industries”.
USEPA, Method 430., “Determination of formaldehyde and acetaldehyde in emission s from stationary sources.”
USEPA, Method 8315A., “Determination of carbonyl compounds by high performance liquid chromatography (HPLC)”.
Uchiyama S, Matsushima E, Aoyagi S, Ando M., Simultaneous, “Determination of C1-C4 carboxylic acids and aldehydes using 2,4-dinitrophenylhydrazine-Impregnated Silica gel and High-Performance Liquid Chromatography”, Anal. Chem. 76:5849-5854., 2004
行政院環境保護署,大氣中有機汙染物質檢驗方法之建立-第二年,EPA-81-E3S3-09-01。(81年)
行政院環境保護署,煙道排氣中醛類檢測方法之驗證與研究,EPA-86-1304-01-01。(86年)
行政院環境保護署,NIEA A705.11C.空氣中氣態之醛類化合物檢驗方法-以 DNPH 衍生物之高效能液相層析測定法。
行政院環境保護署,NIEA A710.10T.空氣中氣態有機溶劑檢驗方法—以活性碳吸附之氣相層析/火焰離子化偵測法。
行政院環境保護署,NIEA A711.1.煙道排氣及周界空氣中C1至C5醛類DNPH衍生物(暫行)之高效能液相層析測定法。
行政院環境保護署,NIEA A715.12B. 空氣中揮發性有機化合物檢測方法-不�袗�採樣筒╱氣相層析質譜儀法。
行政院環境保護署,NIEA A724.72B.排放管道中甲醛標準檢測方法—4-胺基-3-胼基-5-硫醇基-1,2,4-三唑比色法。
行政院環境保護署,NIEA A725.71B.排放管道中醛類標準檢測方法—2,4-二硝基苯胼-高效能液相層析法。
標準分析參考方法-甲醛. 行政院勞委會. http://www.iosh.gov.tw/data/f10/oldcla/cla2403.htm
標準分析參考方法-丙酮.行政院勞委會. http://www.iosh.gov.tw/data/f10/old1211_2.htm
標準分析參考方法-甲基異丁酮. 行政院勞委會.
http://www.iosh.gov.tw/data/f10/cla1211.pdf
連結至畢業學校之論文網頁點我開啟連結
註: 此連結為研究生畢業學校所提供,不一定有電子全文可供下載,若連結有誤,請點選上方之〝勘誤回報〞功能,我們會盡快修正,謝謝!
QRCODE
 
 
 
 
 
                                                                                                                                                                                                                                                                                                                                                                                                               
第一頁 上一頁 下一頁 最後一頁 top