肺癌呼吸检测的电子鼻设计
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摘要
本课题根据国外关于呼吸气体中某些有机气体成分和肺癌相关性的研究工作报告，采用固相微萃取—气相色谱系统对肺癌病人呼吸气体、正常人呼吸气体、和其它类肺病患者呼吸气体中的有机气体成分进行对比检测、研究，以期确定肺癌病人呼吸气体中特征有机气体成分；并且期望建立首创的采用毛细管色谱柱与声表面波传感器联用技术的电子鼻系统，与固相微萃取—气相色谱系统作为对比检测，能够做到粗筛肺癌病人。
在本论文中主要论述的是已经完成的以下两部分工作：
首先介绍了呼吸检测和肺癌呼吸检测的重要性和研究依据，所采用的固相微萃取对有机气体成分的预富集技术，和气相色谱分析有机气体成分的原理；配制标样气体对固相微萃取—气相色谱系统进行定性和定量的标定；然后应用固相微萃取—气相色谱系统对比检测了15例肺癌病人呼吸气体，10例正常人呼吸气体和7例慢性支气管炎病人呼吸气体，基本完成了对肺癌病人呼吸气体中特征有机气体成分的分析。
其次介绍了电子鼻应用于呼吸检测的可行性，涂膜的原理，并通过详细介绍传感器设计、电路设计、软件设计、传感器涂膜和系统设计等方面说明了我们所建立的毛细管色谱柱与声表面波传感器联用电子鼻系统。目前基本完成了标样气体对声表面波传感器的标定，和对毛细管色谱柱与声表面波传感器联用系统的标定及分析。
通过以上工作，为今后通过毛细管色谱柱与声表面波传感器联用电子鼻系统，检测人体呼吸气体中的特征有机气体成分，能够做到基本筛选肺癌病人打下良好、坚实的基础。
This work mainly compared the VOCs in lung cancer patients breath and in normal human breath to determine the correlation between lung cancer and the marker VOCs. Following, we developed an electronic nose adopting advanced technology which combined capillary column to separate VOCs according their different retention time and surface acoustic wave sensor coating with polymer film to detect the qualities of those VOCs.
In my article, lung cancer situation, breath detection principle, feasibility of electronic nose adopting breath detection, and the principles of SPME & GC have been particularly introduced. And initially certified the correlation between lung cancer and the marker VOCs by detecting lung cancer patients breath, normal human breath, and lung problem patients by solid phase microextraction(SPME) and gas chromatography(GC) system. And we mainly finished breath detection electronic nose system, including surface acoustic wave sensor design, film coating design, and hardware & software design for future detection marker VOCs in lung cancer breath by electronic nose.
在本论文中主要论述的是已经完成的以下两部分工作：
首先介绍了呼吸检测和肺癌呼吸检测的重要性和研究依据，所采用的固相微萃取对有机气体成分的预富集技术，和气相色谱分析有机气体成分的原理；配制标样气体对固相微萃取—气相色谱系统进行定性和定量的标定；然后应用固相微萃取—气相色谱系统对比检测了15例肺癌病人呼吸气体，10例正常人呼吸气体和7例慢性支气管炎病人呼吸气体，基本完成了对肺癌病人呼吸气体中特征有机气体成分的分析。
其次介绍了电子鼻应用于呼吸检测的可行性，涂膜的原理，并通过详细介绍传感器设计、电路设计、软件设计、传感器涂膜和系统设计等方面说明了我们所建立的毛细管色谱柱与声表面波传感器联用电子鼻系统。目前基本完成了标样气体对声表面波传感器的标定，和对毛细管色谱柱与声表面波传感器联用系统的标定及分析。
通过以上工作，为今后通过毛细管色谱柱与声表面波传感器联用电子鼻系统，检测人体呼吸气体中的特征有机气体成分，能够做到基本筛选肺癌病人打下良好、坚实的基础。
This work mainly compared the VOCs in lung cancer patients breath and in normal human breath to determine the correlation between lung cancer and the marker VOCs. Following, we developed an electronic nose adopting advanced technology which combined capillary column to separate VOCs according their different retention time and surface acoustic wave sensor coating with polymer film to detect the qualities of those VOCs.
In my article, lung cancer situation, breath detection principle, feasibility of electronic nose adopting breath detection, and the principles of SPME & GC have been particularly introduced. And initially certified the correlation between lung cancer and the marker VOCs by detecting lung cancer patients breath, normal human breath, and lung problem patients by solid phase microextraction(SPME) and gas chromatography(GC) system. And we mainly finished breath detection electronic nose system, including surface acoustic wave sensor design, film coating design, and hardware & software design for future detection marker VOCs in lung cancer breath by electronic nose.
引文
[1] 吴小和，肺癌，江西科学技术出版社，2000年6月第一版
[2] Michael Phillips, Kevin Gleeson, J Michael B Hughes, Joel Greenberg, Renee N Cataneo, Leigh Baker, W Patrick McVay, Volatile organic compounds in breath as markers of lung cancer:a cross-sectional study,Lancet 1999; 353:1930-33
[3] Corrado Di Natale, Antonella Macagnano, Eugenio Martinelli, Lung cancer identification by the analysis of breath by means of an array of non-selective gas sensors, Biosensors and Bioelectronics 18 (2003) 1209_1218
[4] Detlev Helmig, Review Air analysis by gas chromatography, Journal of Chromatography A, 843 (1999) 129-146
[5] 杨姝，叶险峰，鲍春阳，祝铁军，气相色谱法测定大气中超痕量烃(cz—c11)的含量，化学工程师，69(1998)30—32
[6] Gianrico Castello, Maurizio Benzo, Tomaso C. Gerbino, Automated gas chromatographic analysis of volatile organic compounds in air, Journal of Chromatography A. 710(1995)61-70
[7] (美)M．L．李，F．J．杨，K．D．巴特尔，毛细管柱气相色谱法，化学工业出版社，1988年10月第一版
[8] J.C.Giddings, Dynamics of Chromatography, Marce Dekker, New York, 1965
[9] J.H.Purnell, Gas Chromatography John Wiley&Sons. New York, 1967.
[10] 张达英，分析仪器，全国轻化工类高等学校工业分析专业系列教材，1990年6月第一版
[11] Pauling L, Quantitative analysis of urine vapor and breath by gas-liquid partition chromatography. Proc Nat Acad Sci USA 1971;68:2374-2376
[12] Krotozynski, B. K.; Gabriel, G.; O'Neill, H.J.Chromatogr. Sci. 1977, 15:239-244
[13] 沈学优，罗晓璐，空气中挥发性有机物监测技术的研究进展，环境污染与防治第24卷第1期2002年2月
[14] 陈楚良，热解吸—气相色谱分析法，化工劳动保护，1992年第13卷第4期
[15] Alltech Associates, Inc., Gas Sampling Bags, Data Sheet 4150D
[16] Arthur C L, Pawliszyn J, Anal.Chem, 1990,62:2145-2148
[17] Heather Lord, Janusz Pawliszyn, Evolution of solid-phase microextraction technology, Journal of Chromatography A, 885(2000) 153-193
[18] Maria Llompart, Ken Li, Merv Ringas, Headspace solid phase microextraction (HSSPME) for the determination of volatile and semivolatile pollutants in soils, Talanta 48(1999) 451-459
[19] Alexandre Bene, Antonie Fornage, Jean-Luc Luisier, Peter Pichler, Jean-Claude Villettaz, A new method for the rapid determination of volatile substances: the SPME-direct method Part Ⅰ: Apparatus and working conditions, Sensors and Actuators B 72(2001) 184-187
[20] Meng Chai, Janusz Pawliszyn, Analysis of Environmental Air Samples by Solid-Phase Microextraction and Gas Chromatography/Ion Trap Mass Spectrometry, Environ.Sci, Technol, 1995,29,693-701
[21] Christoph Grote, Janusz Pawliszyn, Solid-Phase Microextraction for the Analysis of Human Breath, Anal.Chem, 1997,69,587-596
[22] William A.Groves, Edward T.Zellers, Gregory C.Frye, Analyzing organic vapors in exhaled breath using a surface acoustic wave sensor array with preconcentration: Selection and characterization of the preconcentrator adsorbent, Analytica Chimica Acta 371(1998) 131-143
[23] Wang ping, Tan yi,et al,A novel method for diabetes diagnosis based on slectronics nose, Biosensors & Bioelectronics,Vol 12,No.9-10,1997,pp, 1031-1036
[24] N.RMakksimovich and L.E.Yeremina, Device with semiconductor gas sensor for alcohol vapor detection in an exhaled air sample, Sensors and Actuators B, 13-14,1993,256-258
[25] J.W.Gardner et al, Prediction of bacteria type and culture growth phase by an electronic nose with a multi-layer perception network, Means, Sci&Tech, 9,1998,120-127
[26] 李翼，姚哲钢，浙江大学硕士论文
[27] N. Makisimovich, V. Vorotyntsev N. Nikitina a, O. Kaskevich P. Karabun, F. Martynenko, Adsorption semiconductor sensor for diabetic ketoacidosis diagnosis,
Sensors and Actuators B 35-36 (1996) 419-421
[28] G. Watson, W. Horton, E. Staples, Gas chromatography utilizing SAW sensors, Ultrasonics Symposium, 305-309
[29] 武以立 邓盛刚，王永德，声表面波原理及其在电子技术中的应用，国防工业出版社，1983年8月第一版
[30] Michael J, Vellekoop, Acoustic wave sensors and their technology, Ultrasonics, 36,(1998),7-14
[31] (日)清水刚夫著，李福绵，陈双基翻译，新功能膜，北京联合大学出版社，1990年3月第一版
[32] KentS.Knaebel, adsorbent selection, Adsorption, Research, Inc.Dublin, Ohio 43016
[33] Dunbar R Birnie et al, the key stages in spin coating, J. Imaging Technology 13(1987) 122.
[34] Waldemar Soluch, Design of SAW delay lines for senors, Sensors and Actuators A 67(1998) 60-64
[35] G.Watson, W.Horton, E.Staples, Gas Chromatography Utilizing SAW Sensors, Ultrasonics Symposum, 1999,305-309
[36] E. J. Staples and G.W. Watson, A GAS Chromatograph Incorporating an Innovative New Surface Acoustic Wave (SAW) Detector, Pittcon Conference.
[37] Edward J. Staples, The zNose, A New Electronic Nose Using Acoustic Technology, Acoustical Society of America, December 2000, Paper No: 2aEA4 1-5 March 1998, New Orleans, Louisiana, Paper No: 1583CP
[38] Edward J. Staples, The First Quantitatively Validated Electronic Nose for Environmental Test of Air, Water, and Soil, American Chemical Society, ACS National, Marth 26-30,2000
[39] T.Nakamoto, T.Morizumi, Artificial olfactory system using neural network, Handbook of Sensors and Acutuators, Vol.3, 1996,263-272
[2] Michael Phillips, Kevin Gleeson, J Michael B Hughes, Joel Greenberg, Renee N Cataneo, Leigh Baker, W Patrick McVay, Volatile organic compounds in breath as markers of lung cancer:a cross-sectional study,Lancet 1999; 353:1930-33
[3] Corrado Di Natale, Antonella Macagnano, Eugenio Martinelli, Lung cancer identification by the analysis of breath by means of an array of non-selective gas sensors, Biosensors and Bioelectronics 18 (2003) 1209_1218
[4] Detlev Helmig, Review Air analysis by gas chromatography, Journal of Chromatography A, 843 (1999) 129-146
[5] 杨姝，叶险峰，鲍春阳，祝铁军，气相色谱法测定大气中超痕量烃(cz—c11)的含量，化学工程师，69(1998)30—32
[6] Gianrico Castello, Maurizio Benzo, Tomaso C. Gerbino, Automated gas chromatographic analysis of volatile organic compounds in air, Journal of Chromatography A. 710(1995)61-70
[7] (美)M．L．李，F．J．杨，K．D．巴特尔，毛细管柱气相色谱法，化学工业出版社，1988年10月第一版
[8] J.C.Giddings, Dynamics of Chromatography, Marce Dekker, New York, 1965
[9] J.H.Purnell, Gas Chromatography John Wiley&Sons. New York, 1967.
[10] 张达英，分析仪器，全国轻化工类高等学校工业分析专业系列教材，1990年6月第一版
[11] Pauling L, Quantitative analysis of urine vapor and breath by gas-liquid partition chromatography. Proc Nat Acad Sci USA 1971;68:2374-2376
[12] Krotozynski, B. K.; Gabriel, G.; O'Neill, H.J.Chromatogr. Sci. 1977, 15:239-244
[13] 沈学优，罗晓璐，空气中挥发性有机物监测技术的研究进展，环境污染与防治第24卷第1期2002年2月
[14] 陈楚良，热解吸—气相色谱分析法，化工劳动保护，1992年第13卷第4期
[15] Alltech Associates, Inc., Gas Sampling Bags, Data Sheet 4150D
[16] Arthur C L, Pawliszyn J, Anal.Chem, 1990,62:2145-2148
[17] Heather Lord, Janusz Pawliszyn, Evolution of solid-phase microextraction technology, Journal of Chromatography A, 885(2000) 153-193
[18] Maria Llompart, Ken Li, Merv Ringas, Headspace solid phase microextraction (HSSPME) for the determination of volatile and semivolatile pollutants in soils, Talanta 48(1999) 451-459
[19] Alexandre Bene, Antonie Fornage, Jean-Luc Luisier, Peter Pichler, Jean-Claude Villettaz, A new method for the rapid determination of volatile substances: the SPME-direct method Part Ⅰ: Apparatus and working conditions, Sensors and Actuators B 72(2001) 184-187
[20] Meng Chai, Janusz Pawliszyn, Analysis of Environmental Air Samples by Solid-Phase Microextraction and Gas Chromatography/Ion Trap Mass Spectrometry, Environ.Sci, Technol, 1995,29,693-701
[21] Christoph Grote, Janusz Pawliszyn, Solid-Phase Microextraction for the Analysis of Human Breath, Anal.Chem, 1997,69,587-596
[22] William A.Groves, Edward T.Zellers, Gregory C.Frye, Analyzing organic vapors in exhaled breath using a surface acoustic wave sensor array with preconcentration: Selection and characterization of the preconcentrator adsorbent, Analytica Chimica Acta 371(1998) 131-143
[23] Wang ping, Tan yi,et al,A novel method for diabetes diagnosis based on slectronics nose, Biosensors & Bioelectronics,Vol 12,No.9-10,1997,pp, 1031-1036
[24] N.RMakksimovich and L.E.Yeremina, Device with semiconductor gas sensor for alcohol vapor detection in an exhaled air sample, Sensors and Actuators B, 13-14,1993,256-258
[25] J.W.Gardner et al, Prediction of bacteria type and culture growth phase by an electronic nose with a multi-layer perception network, Means, Sci&Tech, 9,1998,120-127
[26] 李翼，姚哲钢，浙江大学硕士论文
[27] N. Makisimovich, V. Vorotyntsev N. Nikitina a, O. Kaskevich P. Karabun, F. Martynenko, Adsorption semiconductor sensor for diabetic ketoacidosis diagnosis,
Sensors and Actuators B 35-36 (1996) 419-421
[28] G. Watson, W. Horton, E. Staples, Gas chromatography utilizing SAW sensors, Ultrasonics Symposium, 305-309
[29] 武以立 邓盛刚，王永德，声表面波原理及其在电子技术中的应用，国防工业出版社，1983年8月第一版
[30] Michael J, Vellekoop, Acoustic wave sensors and their technology, Ultrasonics, 36,(1998),7-14
[31] (日)清水刚夫著，李福绵，陈双基翻译，新功能膜，北京联合大学出版社，1990年3月第一版
[32] KentS.Knaebel, adsorbent selection, Adsorption, Research, Inc.Dublin, Ohio 43016
[33] Dunbar R Birnie et al, the key stages in spin coating, J. Imaging Technology 13(1987) 122.
[34] Waldemar Soluch, Design of SAW delay lines for senors, Sensors and Actuators A 67(1998) 60-64
[35] G.Watson, W.Horton, E.Staples, Gas Chromatography Utilizing SAW Sensors, Ultrasonics Symposum, 1999,305-309
[36] E. J. Staples and G.W. Watson, A GAS Chromatograph Incorporating an Innovative New Surface Acoustic Wave (SAW) Detector, Pittcon Conference.
[37] Edward J. Staples, The zNose, A New Electronic Nose Using Acoustic Technology, Acoustical Society of America, December 2000, Paper No: 2aEA4 1-5 March 1998, New Orleans, Louisiana, Paper No: 1583CP
[38] Edward J. Staples, The First Quantitatively Validated Electronic Nose for Environmental Test of Air, Water, and Soil, American Chemical Society, ACS National, Marth 26-30,2000
[39] T.Nakamoto, T.Morizumi, Artificial olfactory system using neural network, Handbook of Sensors and Acutuators, Vol.3, 1996,263-272