Polymer films as sensitive coatings for quartz crystal microbalance sensors array

This work reports on the results of investigation of quarts crystal microbalance sensors coated with polybutyl methacrylate and polyvinyl formal/ethylal to wide range of volatile organic compounds. Polymer film coated sensors showed a high sensitivity and an excellent selectivity towards these compo...

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Опубліковано в: :Semiconductor Physics Quantum Electronics & Optoelectronics
Дата:2003
Автори: Koshets, I.A., Kazantseva, Z.I., Shirshov, Yu.M.
Формат: Стаття
Мова:Англійська
Опубліковано: Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України 2003
Онлайн доступ:https://nasplib.isofts.kiev.ua/handle/123456789/118076
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Цитувати:Polymer films as sensitive coatings for quartz crystal microbalance sensors array / I.A. Koshets, Z.I. Kazantseva, Yu.M. Shirshov // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2003. — Т. 6, № 4. — С. 505-507. — Бібліогр.: 8 назв. — англ.

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Digital Library of Periodicals of National Academy of Sciences of Ukraine
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author Koshets, I.A.
Kazantseva, Z.I.
Shirshov, Yu.M.
author_facet Koshets, I.A.
Kazantseva, Z.I.
Shirshov, Yu.M.
citation_txt Polymer films as sensitive coatings for quartz crystal microbalance sensors array / I.A. Koshets, Z.I. Kazantseva, Yu.M. Shirshov // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2003. — Т. 6, № 4. — С. 505-507. — Бібліогр.: 8 назв. — англ.
collection DSpace DC
container_title Semiconductor Physics Quantum Electronics & Optoelectronics
description This work reports on the results of investigation of quarts crystal microbalance sensors coated with polybutyl methacrylate and polyvinyl formal/ethylal to wide range of volatile organic compounds. Polymer film coated sensors showed a high sensitivity and an excellent selectivity towards these compounds. Good linearity of the concentration dependence has been obtained in almost all the concentration range of volatile compounds. The detection limit of several analytes was less than 100 ppm.
first_indexed 2025-12-07T15:59:02Z
format Article
fulltext 505© 2003, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine Semiconductor Physics, Quantum Electronics & Optoelectronics. 2003. V. 6, N 4. P. 505-507. PACS: 07.07.Df Polymer films as sensitive coatings for quartz crystal microbalance sensors array I.A. Koshets, Z.I. Kazantseva, Yu.M. Shirshov V. Lashkaryov Institute of Semiconductor Physics, NAS of Ukraine, 41, prospect Nauky, 03028 Kyiv, Ukraine E-mail: koshets@isp.kiev.ua Abstract. This work reports on the results of investigation of quarts crystal microbalance sensors coated with polybutyl methacrylate and polyvinyl formal/ethylal to wide range of volatile organic compounds. Polymer film coated sensors showed a high sensitivity and an excellent selectivity towards these compounds. Good linearity of the concentration depend- ence has been obtained in almost all the concentration range of volatile compounds. The detection limit of several analytes was less than 100 ppm. Keywords: quartz crystal microbalance sensor, polymer coating, volatile organic compounds. Paper received 06.11.03; accepted for publication 11.12.03. 1. Introduction Nowadays a great attention is paid to creation and de- velopment of miniaturized, low-cost, smart chemical sens- ing systems based on various physical and chemical prin- ciples, which provide accurate and reliable real-time con- trol of ambient medium [1�2]. One of the most important problems under creation of such systems (known as �Elec- tronic noses�) for pattern recognition of smells is the choice of appropriate sensitive materials used as coat- ings of such a sensor. Requirements that should be met with these layers are quite versatile and even con- tradictious. On the one hand, the sensor should provide good and quick response to the presence of analyzed molecules in ambient air, on the other hand, the sensor must have sensitivity to the interfering molecules as less as possible. Besides, the sensor should be easily cleaned. From this viewpoint, various types of polymers are very promising materials, and many researchers focus their attention on investigations of selective and sensitive prop- erties of polymer films [3�5]. This work is aimed at the study of polybutyl methacrylate (PBMA) and polyvinyl formal ethylal (PVFE) as sensitive layers for (quarts crys- tal microbalance) QCM sensor. 2. Experimental The basis of QCM technique is the proportionality be- tween mass loaded onto quartz surface and oscillations frequency shifts in according to the Sauerbrey equation [6]. So, measuring the frequency shift, one can easily investigate adsorption-desorption processes occurring at onto sensor surface. Sensitivity of this method is very high � 1�2 ng/Hz, which allows detecting the very low concen- tration of organic vapors. 8-channel QCM sensor system with all the necessary equipment (gas cell, gas-supplying system and electronic circuits, etc.) designed in our labo- ratory has been used in experiments. The experiment con- trol and data acquisition were implemented with PC by means of domestic software. Gas-supplying regime cho- sen for our experiments was of non-flow type: after rap- idly injected analyte gas, the cell was cut off from pipe- line and no gas flow occured during the measuring pe- riod. The detailed description of this device and gas sup- plying regime can be found in [7]. Polymers were deposited onto quarts surface by means of dipping and spin coating techniques. Information about morphology and determination of the thickness of layers deposited has been was obtained from ellipsometry and AFM measurements. The average film thickness was about 50-70 nm (on each side of quartz sensor), which corresponds to 2000-3000 Hz frequency shift. After depo- sition, sensors were dried with fresh dry air for 12-15 hours to draw out the remaining solvent from coatings. Chemical structures of polymers are shown in Fig. 1. Such volatile organic compounds as chlorbenzene (C6H5Cl), benzene (C6H6), toluene (C7H8), dichloro- methane (CH2Cl2), carbon tetrachloride (CCl4), chloro- form (CHCl3) and ethanol (C2H6O) were involved in our 506 SQO, 6(4), 2003 I.A. Koshets et al.: Polymer films as sensitive coatings for quartz crystal ... experiments. The required concentration was provided with the home made vapor generating system based on the diffusion tube principle [8]. 3. Results and discussion Typical kinetics of sensors response to injection of differ- ent organic vapors (ethanol, dichloromethane and chlo- robenzene) is presented in Fig. 2. Numbers in plots de- note the concentration of analyte. Two types of the curve shape are observed: the first one � gradual (�slow�) changing of the frequency shift followed by the flat part of the curve; the second � �fast� response with pronounced maximum followed by a dip of the curve. Such distinct behavior strongly depends on correlation of such factors as gas cell capacity, initial number of volatile molecules injected, numbers of sensors and cell sites, and their time constants (�slow� or �fast� they are). The detailed de- scription of this phenomenon can be found in [2]. It was found that PMBA film coated sensor exhibited a high sensitivity and an excellent selectivity for chlorbenzene, although the sensor also responded to chlo- roform, chlormethelene and toluene, responses towards alcohol were insignificant. The responses of PVFE film coated show a high sensitivity towards alcohol but low sensitivity towards chlorine organic vapors. In some cases, e.g. chlormethelene, magnitude of response is similar for two polymers, but the shape of kinetic curve strongly dif- ferent. It provides us extra information for goals of pat- tern recognition. As known, selective features of organic sensitive layer mainly coincide with solubility parameter towards or- ganic solvents [1]. In other words, the closer solubility parameters of given organic layer and given solvent, the higher response of the sensor coated with this layer to the vapor of that solvent. For example, solubility parameters of PBMA are closer to those of benzene and chlorbenzene but smaller than that of ethanol. Similar situation is ob- served in QCM measurements � sensor coated with PBMA shows maximal response to carbon tetrachloride vapor. Although, situation is more complicated for copolymers (PFE) consisting of different polarity monomers. In this case, the dipole�dipole interaction plays a significant role, which should be taken into account for analysis of sensing features inherent to these coatings. Concentration dependencies extracted from kinetic curves are shown in Fig. 3. Good linearity is seen almost over all the concentration range of analytes. 0 200 400 600 800 1000 �40 �30 �20 �10 0 10 PBMA PVFE 10000 5000 3000 2000 1000 600 300 ∆ f, H z time, s a 0 200 400 600 800 1000 �60 �40 �20 0 PBMA PVFE 500 1000 2000 4000 8000 16000 ∆ f, H z time, s b 0 200 400 600 800 1000 �60 �40 �20 0 PBMA PVFE 100 200 300 500 1000 2000 ∆ f, H z time, s c Fig. 2. Kinetic response (frequency shift) of sensors coated with polymers to injection of ethanol (a), dichloromethane (b) and chlorbenzene (c) vapor. a [C � CH2 ] N  O = C � O � (CH2)3 � CH3 b [CH � CH2 � CH � CH2 ]X [CH2 � CH ]Y    O � CH � O OH  CH3 [CH2 � CH ]Z  OCOCH3 Fig. 1. Chemical structure of polymers: a) � PBMA; b) � PVFE. I.A. Koshets et al.: Polymer films as sensitive coatings for quartz crystal ... 507SQO, 6(4), 2003 Table.1. Sensitivity and detection threshold of sensors coated with PBMA and PVFE. Volatile organic PBMA PVFE molecules Sensitivity, Detection Sensitivity, Detection 10�4×Hz/ppm threshold, ppm 10�4×Hz/ppm threshold, ppm Benzene 38.8 300 10.8 <300 Ethanol 9.34  2000 34 <300 Toluene 87.7  <250 10.5 <500 Carbon tetrachloride 86  <500 5.92 2000 Chloroform 93.4  <300  8.5  500 Dichloromethane 36 500 24  500 Chlorobenzene 34.5  <100 17.1 2000 0 3000 6000 9000 12000 15000 �60 �50 �40 �30 �20 �10 0 ∆ f, H z concentration, ppm Benz Eth Tol CCl4 Clor ClMet ClBen a 0 3000 9000 15000 �30 �25 �20 �15 �10 �5 0 ∆ f, H z concentration, ppm b Benz Eth Tol CCl4 Clor ClMet ClBen Fig. 3. Sensitivity of sensors coated with PBMA (a) and PVFE (b) towards various volatile organic molecules. Slightly sublinear shape of curves in the high concentra- tion level (one or two last points) might be related to satura- tion of sensitive sites in the film. Numerical values of the sensitivity and detection limit are presented in Table1. Sensors coated with PBMA and PVFE accompanied with sensors coated with other polymers were combined into array that was successfully tested for discrimination of wide number of aromatic and chlororganic volatile compounds and several items of brandy produced in Ukraine. 4. Conclusions Summarizing all mentioned above, we may conclude that polymer and copolymer are promising materials for us- ing them as a sensitive layer of sensors elements in a chemical sensing system. Varying functional groups of polymer, we can find appropriate set of sensors for reli- able recognition of volatile organic compounds in ambi- ent atmosphere and testing the quality of alcohol bever- ages, perfumes, etc. Application of statistical apparatus (PCA, Neural Network, etc.) to data obtained from the sensor array allows increasing such recognition. References 1. Ch. Ziegler, W. Gopel, at all, Bioelectronic noses: a status report. Part I // Biosensors & Bioelectronics, 13 (3-4), pp.479- 493 (1998). 2. Ch. Ziegler, W. Gopel, at all, Bioelectronic noses: a status re- port. Part II // Biosensors & Bioelectronics, 13, pp. 539-571 (1998). 3. S.Roster, R.Lucklum, R.Borngraber, J.Hartmann, P.Haupt- mann, Sensor system for the detecion of organic pollutants in water by thickness shear mode resonators // Sensors & Ac- tuators. B 48, pp. 412-424 (1998). 4. R.Polikar, R.Shinar, L.Udpa, M.D.Porter, Artificial intelli- gent methods of an optimized sensor array for identification of volatile organic compounds // Sensor & Actuators, B 80, pp.243-254 (2001). 5. H. Nanto, Y. Yokoi, T. Mukai, J. Fujioka, E. Kusano, A. Kinbara, Y. Douguchi, Novel gas sensor using polymer- film-coated quartz resonator for environment monitorinq // Material Science and Engineering, C-21, pp. 43-48 (2000). 6. F.Eichelbaum, R. Borngraber, J. Schroder, R. Lucklum and P. Hauptmann, Interface circuits for QCM sensors // Review of Scientific Instruments, 70, May, 1999. 7. V.I.Kalchenko, I.A.Koshets, E.P.Matsas, O.N.Kopylov, A.Solovyov, Z.I. Kazantseva, Yu.M.Shirshov, Calixarene based QCM sensors array and its response to volatile or- ganic vapors// Materials Science, 20 (3), pp.73-88 (2002). 8. J.M. McKelvey and H.E. Hoelscher, Apparatus for prepa- ration of very dilute gas mixtures // Analytical chemistry, 29 (1), pp.123-124 (1957).
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institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
issn 1560-8034
language English
last_indexed 2025-12-07T15:59:02Z
publishDate 2003
publisher Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
record_format dspace
spelling Koshets, I.A.
Kazantseva, Z.I.
Shirshov, Yu.M.
2017-05-28T16:34:48Z
2017-05-28T16:34:48Z
2003
Polymer films as sensitive coatings for quartz crystal microbalance sensors array / I.A. Koshets, Z.I. Kazantseva, Yu.M. Shirshov // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2003. — Т. 6, № 4. — С. 505-507. — Бібліогр.: 8 назв. — англ.
1560-8034
PACS: 07.07.Df
https://nasplib.isofts.kiev.ua/handle/123456789/118076
This work reports on the results of investigation of quarts crystal microbalance sensors coated with polybutyl methacrylate and polyvinyl formal/ethylal to wide range of volatile organic compounds. Polymer film coated sensors showed a high sensitivity and an excellent selectivity towards these compounds. Good linearity of the concentration dependence has been obtained in almost all the concentration range of volatile compounds. The detection limit of several analytes was less than 100 ppm.
en
Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
Semiconductor Physics Quantum Electronics & Optoelectronics
Polymer films as sensitive coatings for quartz crystal microbalance sensors array
Article
published earlier
spellingShingle Polymer films as sensitive coatings for quartz crystal microbalance sensors array
Koshets, I.A.
Kazantseva, Z.I.
Shirshov, Yu.M.
title Polymer films as sensitive coatings for quartz crystal microbalance sensors array
title_full Polymer films as sensitive coatings for quartz crystal microbalance sensors array
title_fullStr Polymer films as sensitive coatings for quartz crystal microbalance sensors array
title_full_unstemmed Polymer films as sensitive coatings for quartz crystal microbalance sensors array
title_short Polymer films as sensitive coatings for quartz crystal microbalance sensors array
title_sort polymer films as sensitive coatings for quartz crystal microbalance sensors array
url https://nasplib.isofts.kiev.ua/handle/123456789/118076
work_keys_str_mv AT koshetsia polymerfilmsassensitivecoatingsforquartzcrystalmicrobalancesensorsarray
AT kazantsevazi polymerfilmsassensitivecoatingsforquartzcrystalmicrobalancesensorsarray
AT shirshovyum polymerfilmsassensitivecoatingsforquartzcrystalmicrobalancesensorsarray