Vol. 8, Supplement A (1992)
Digest of the 14th Chemical Sensor Symposium
April 2-4, 1992
Tokyo Metropolitan University
Abstracts
1
アポ酵素膜を用いた銅(II)イオンのフローアンペロメトリックバイオセンシング
佐藤生男・安西広行・伊藤 肇
神奈川工科大工
FLOW-AMPEROMETRIC BIOSENSING OF COPPER (II)
IONS USING AN APOENZYME-MEMBRANE
Ikuo SATOH, Hiroyuki ANZAI and Hajime ITOH
Department of Chemical Technology, Faculty of Engineering, Kanagawa Institute of Technology
1030 Shimo-Ogino, Atsugi-shi, Kanagawa 243-02, Japan
Ascorbate oxidase covalently immobilized onto a porous polymer membrane is used as the recognition element for copper(II) ions. The biosensing system is assembled with the enzyme-membrane attached onto an oxygen electrode housed in a flow-through cell for monitoring the enzymic activity. Copper(II) ions are amperometrically determined in 5.0 to 50 μM through its activation of the immobilized metal-free enzyme (apoenzyme). The activity is assessed by injecting a 0.1 ml of 10 mM L-ascorbate as the substrate and thereby, the change in oxygen uptake due to the enzymic reaction is measured. The membrane is regenerated by pumping N,N-diethyldithiocarbamate solution (pH 8.0).
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2
L -アスコルビン酸とデヒドロアスコルビン酸のサイクリック反応を利用する高感度ビタミンCセンサ
内山俊一・鈴木周一
埼玉工大工
HIGHLY SENSITIVE VITAMIN C SENSOR USING THE CYCLIC REACTION BETWEEN L-ASCORBIC ACID AND DEHYDROASCORBIC ACID
Shunichi UCHIYAMA and Shuichi SUZUKI
Department of Environmental Engineering, Saitama Institute of Technology
Okabe, Saitama 369-02, Japan
A cyclic reaction between the reduced and the oxidized forms of Vitamin C takes place by combining the ascorbate oxidase reaction and the reduction of L-ascorbic acid to dehydroascorbic acid by dithiothreithol. L-ascorbic acid is oxidized by the dissolved oxygen and its consumption is not compensated by the chemical regeneration of L-ascorbic acid from dehydroascorbic acid. The dissolved oxygen then continues to decrease during the cyclic reaction, consequently, the decrease of the reduction current of oxygen is amplified. In the batch system, the amplification factor of 5×10-5 M L-ascorbic acid at 5×10-3 M dithiothreithol and pH 7.5 was found to be 10.6 ehen enzyme activity is 0.64 Units/ml and the reaction time is 10 minutes. The amplification factor was increased up to 22 when the immobilized ascorbate oxidase membrane electrode was employed. The present method enables the measurement of not only L-ascorbic acid but also dehydroascorbic acid and the total vitamin C can be easily determined.
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3
脱水素酵素／NADH酸化酵素を利用したセンサ系によるD-,L-乳酸の同時測定
水谷文雄・矢吹聡一・曽良達生
繊高研
SIMULTANEOUS DETERMINATION OF D-LACTATE AND L-LACTATE WITH A TWO-ELECTRODE SENSOR SYSTEM
Fumio MIZUTANI, Soichi YABUKI and Tatsuo KATSURA
Research Institute for Polymers and Textiles
1-14 Higashi, Tsukuba, Ibaraki 305, Japan
A D-lactate-sensing electrode was constructed from an oxygen electrode and a layer containing immobolized D-lactate dehydrogenase (D-LDH) and NADH oxidase, and an L-lactate-sensing one, from an oxygen electrode and a layer containing L-lactate dehydrogenase (L-LDH) and NADH oxidase. Each electrode was stable for more than 4 weeks. A two-electrode sensor system consisting of the D- and L-lactate-sensing electrodes was prepared and applied to the simultaneous determination of the two components in sour milk.
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4
パルス法におけるEEE型ミクロバイオセンサの応答機構
山内 繁・横山崇裕*・矢尾板仁・碇山義人**
国立リハ研・東京理科大理*・東工大工**
REACTION MECHANISM OF ENZYME EMBODIED ELECTRODE GLUCOSE SENSOR IN POTENTIOSTATIC PULSE RESPONSE
Shigeru YAMAUCHI, Takahiro YOKOYAMA, Masashi YAOITA and Yoshihito IKARIYAMA
Research Institute of National Rehabilitation Center
4-1 Namiki, Tokorozawa, Saitama 359, Japan
Department of Chemistry, Science University of Tokyo
1-3 Kagurazaka, Shinjuku-ku, Tokyo 162, Japan
Dept. of Bioengineering, Tokyo Institute of Technology
4259 Nagatsuda, Midori-ku, Yokohama 227, Japan
A reaction model in the micropores of platinum black is proposed in order to interpret a transient current to a potentiostatic purse on an enzyme embodied electrode glucose sensor, wherein glucose oxidase is immobilized on the platinum black. A steady state in the glucose concentration was assumed, established by a balance of diffusion and oxidation of glucose. Under an open circuit condition concentration of hydrogen peroxide approaches to a steady state by a balance of production and diffusion. Assuming this concentration profile as an initial condition, time-dependence of a transient current to a potentiostatic pulse was calculated. An equation was obtained which exhibited that the current should be proportional to the glucose concentration and exponentially decrease with time. Moreover, the time constant should be independent of glucose concentration. Experimental result supported these deduction and supported the present model.
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5
酵素固定化TCNQ錯体薄膜を用いたグルコースセンサ (2)
岸本芳久・大下佳子
住友金属工業未来技術研
THIN FILM ELECTRODE BASED ON TCNQ COMPLEX AND IMMOBILIZED ENZYME FOR GLUCOSE SENSOR (2)
Yoshihisa KISHIMOTO and Yoshiko OHSHITA
Sumitomo Metal Industries, Ltd. Advanced Technology Research Laboratories
1-8 Fusocho, Amagasaki, Hyogo 660, Japan
Thin film of TCNQ (tetracyanoquinodimethane) complex and immobilized glucose oxidase (GOD) was prepared and the applicability of this new type of enzyme electrode for an amperometric glucose sensor was evaluated.
This enzyme electrode is coated with two layers. The inner layer of the TCNQ charge transfer complex was electrolyzed spontaneously on the surface of Ag substrate in TCNQ solution. In the outer layer there are incorporated GOD and an electron mediator uniformly in the polymer matrix.
The counter electrode is placed near the enzyme electrode and these two electrodes consist a glucose sensing system.
The system shows a rapid current response to the drop of samples without preliminary treatment (diluting or mixing the sample).
Furthermore, the system can be applied to human serum up to 25 mM of glucose.
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6
エポキシ架橋固定化酵素膜を用いたISFET型尿素センサの試作
齋藤 敦・塩野谷紀聖子*・木村 純・栗山敏秀**
日本電気資源研・日本電気分析評価センタ*・日本電気マイクロ研**
DEVELOPMENT OF AN ISFET UREA SENSOR USING EPOXY COMPOUND CROSSLINKING ENZYME MEMBRANE
Atsushi SAITO, Kiseko SHIONOYA*, Jun KIMURA and Toshihide KURIYAMA**
Resources & Environment Protection Research Laboratories
*Analysis & Evaluation Technology Center
**Microelectronics Research Laboratories
NEC Corporation
Kawasaki, kanagawa 216, Japan
An ion-sensitive field-effect transistor (ISFET) urea sensor using ethylene glycol diglycidyl ether (EDGE) as a crosslinking regent was developed and evaluated. The enzyme solution containing bovine serum albumin, glutaraldehyde and EDGE is spin coated onto a silicon on sapphire (SOS)/ISFETs wafer covered with a patterned photoresist. The resulting enzyme membrane is lifted off by ultrasonic vibration in organic solvent, except for the membrane on the ion-sensitive region. Investigation of the membrane by means of 13C NMR indicates EDGE mainly links to carboxyl radical. This sensor shows good storage stability and long term stability comparing with the sensor not including EDGE. This sensor is also applied to measure diluted serum sample. The output shows a good linear relationship with up to 135 mg/dl urea and correlates well by conventional method.
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7
D -アミノ酸オキシダーゼを固定したポリ（メルカプト-p-ベンゾキノン）膜被覆電極のセンサ機能
林 守・新井五郎・安盛岩雄
神奈川大工
POLY (MERCAPTO-p-BENZOQUINONE) CONTAINIG D-AMINO ACID OXIDASE FOR AMPEROMETRIC BIOSENSOR
Mamoru HAYASHI, Gorou ARAI and Iwao YASUMORI
Department of Applied Chemistry, Faculty of Engineering, Kanagawa University
Kanagawa-ku, Yokohama 221, Japan
D-Amino acid oxidase was immobilized in poly (mercapto-p-benzoquinone), a conductive polymer film, on glassy carbon electrode (GCE) by electrochemical polymerization of mercapto-hydroquinone in the presence of the enzyme. The resulting polymer film showed sensitivities and excellent selectivities to D-amino acids when no mediator was used in solution and had good durability when stored in pH 6.4 phosphate buffer solution at ca. 5℃. The polymer-coated GCE had promissing characteristics for apprication to a new type of amperometric D-amino acid sensor, based on dirrect electron transfer from active redox centor in the enzyme, FAD, to GCE via the conductive polymer chain.
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8
酵素包括ポリピロール電極における電荷輸送効率に関する検討
立間 徹・渡辺 毅・權平正幸・渡辺 正
東大生研
CHARGE TRANSFER EFFICIENCY OF ENZYME-INCORPORATED POLYPYRROLE MEMBRANE ELECTRODES
Tetsu TATSUMA, Tsuyoshi WATANABE, Masayuki GONDAIRA and Tadashi WATANABE
Institute of Industrial Science, University of Tokyo
Roppongi, Minato-ku, Tokyo 106, Japan
Though enzyme-incorporated conducting polymer electrodes have been pointed out to enhance the enzyme/electrode charge transfer efficiency owing to close proximity of the electrode to all enzyme molecules, it is difficult to prove this experimentally. It is almost impossible to fabricate two enzyme-incorporated polymer membrane electrodes, by changing the polymer conductivity alone with other parameters kept unchanged. Here we treat this problem by theoretical modeling. The simulated enzyme/electrode charge transfer efficiency of (1) the enzyme electrode model with a conducting polymer on an insulator solid support and (2) that with an insulator polymer on a conducting solid electrode were compared. By use of a common electrode reaction rate constant per surface area, the advantage of the former electrode model was substantiated.
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特別講演１
バイオセンサの新しい応用
軽部征夫
東大先端研
NOVEL APPLICATIONS OF BIOSENSORS
Isao KARUBE
Research Center for Advanced Science and Technology, University of Tolyo
4-6-1 Komaba, Meguro-ku, Tokyo 153, Japan
Many kinds of biosensors have been developed since they were first reported. At present day, biosensors are applied extensively to medical field, food industry, process control and environmental monitoring. In this presentation, novel applications of biosensors are discussed.
We developed a novel protein sensor using a piezoelectric quartz crystal. This can be applied to protein concentration determination in urine.
The highly selective determination of methanol was successfully developed. Methanol was detected by using alcohol oxidase, formaldehyde dehydrogenase and 1-mithoxy-5-mithylphenazinium methylsulfate. Dissolved oxygen was reduced, and hydrogen peroxide generated was measured by using chemiluminescence of lunminol.
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9
ポリピロールを分子インターフェイスとしたNADHの電気化学酸化を利用したアルコール酵素センサ
津島治子・Anwara Begum・篠原寛明・Golamu F. Khan・碇山義人・相澤益男
東工大生命理工
ENZYME SENSOR FOR ALCOHOL WITH NADH-OXIDIZABLE POLYPYRROLE FILM AS MOLECULAR INTER FACE
Haruko TSUSHIMA, Anwara BEGUM, Hiroaki SHINOHARA, Golamu F.KHAN, Yoshihito IKARIYAMA and Masuo AIZAWA
Tokyo Institute of Technology
4259 Nagatsuta, Midori-ku, Yokohama 227, Japan
Electrochemical oxidation of NADH to NAD+ at a polypyrrole-coated Pt electrode was characterized to develop a molecular interface for NAD-requiring enzymes. NADH was oxidized effectively at a potential around 0.4 V on a PF6--doped polypyrrole which was prepared in an organic solvent. Another polypyrrole with other anion doping did not show such significant effect. Alcohol dehydrogenase (ADH) and NAD were then coimmobilized in an ultrathin film on a PF6--doped polypyrrole/Pt electrode by using electrochemical polymerization of pyrrole in 0.1 M KCL solution to fabricate an amperometric enzyme sensor for alcohol. Response current for ethanol by this electrode at 0.4 V was monitored at a given concentration of ethanol. It was considered that the PF 6--doped polypyrrole film works as a molecular interface between reduced NAD and Pt electrode. Ethanol was determined in the concentration range from 20 to 700 mM.
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10
Fabrication of a New Biosensor by Co-immobilizing Enzyme and Organic Conducting Salt in Polypyrrole Matrix
Anwara Begum, Haruko Tsushima, Hiroaki Shinohara, Yoshihito Ikariyama and Masuo Aizawa
Dept. Bioengineering, Tokyo Inst. Tech.
Amperometric enzyme sensors were fabricated by co-immobilizing redox enzymes and organic conducting salt in polypyrrole-interfaced electrodes. In the first step, redox enzyme (glucose oxidase or fructose dehydrogenase) and TTF-TCNQ complex were co-immobilized on a glassy carbon electrode with a dialysis membrane. In the second step, this mixed powder layer was reinforced with a conducting polymer by performing electrochemical polymerization of pyrrole to facilitate the electronic communication and to stabilize the sensor. Specific and benififial sensing for glucose and fructose was carried out by GOD (FAD enzyme) and FDH (PQQ enzyme), respectively. Mixing ratio of the enzyme to the complex and polymerization charge were important factors to obtain eligible sensor response. It was demonstrated that the combination of the organic conducting salt and the conducting polymer works as an effective molicular interface between the redox enzyme and the electrode.
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11
Immobilization of Glucose Oxidase onto Biocompatible Material and Its Application to Fabricate a Needle-Type Glucose Sensor
Chien-Yuan-Chen, Eiichi Tamiya, Kazuhiko Ishihara*, Nobuo Nakabayashi* and Isao Kabube
RCAST, Univ. Tokyo, IMDE Tokyo Med. Dent. Univ.*
A biocompatible copolymer with epoxy group, MBG, was prepared by copolymerization of 2-methacryloyloxyethyl phosphorylcholine (MPC), n-butylmethacrylate (BMA) and glycidylmethacrylate (GMA). This copolymer can immobilize enzyme by a covalent bonding betweenits epoxy group and the amino group of enzyme, Glucose oxidase (GOD) was immobilized by incubating the mixture of GOD and MBG at 37℃ for 3 hours. The GOD-MBG mixture was mixed with cellulose triacetate solution and then dip-coated onto the active surface of the working electrode of the sensor where a Nafion membrane had already been coated. The dynamic range of the sensor was 0-450 mg/dl glucose (0-25 mM). Time needed for 95% response under batch operation was less than 120 seconds. The relative error of the sensor for 24 successive determination of 100 mg/dl glucose solution at 37℃ in PBS was less than 5%. Response of the sensor in control serum maintained stable for 36 hours. This sensor was used to determine glucose in human serum. Data from the sensor showed good agreement with that from a clinical autoanaluzer (r>0.95).
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12
人工膵臓用酸化チタン型グルコースセンサの微少化
池田章一郎・原 将記・伊藤 要
名大工
MINIATURIZATION OF TiO2 TYPE GLUCOSE SENSOR FOR ARTIFICIAL PANCREAS
Shoichiro IKEDA, Masanori HARA and Kaname ITO
Department of Applied Chemistry, Nagoya Institute of Technology
Gokiso-cho, Showa-ku, Nagoya 466, Japan
The needle type titanium oxide glucose sensor for artificial pancreas and the modification of platinum on the titanium oxide surface have been already reported. Miniaturization of the sensor has been performed by using the side wall of the titanium wire (0.3 mm in dia.) electrode as the active and enzyme immobilizing site. The size of the sensor is ca. 1.0 mm in dia. and 15 mm in length except for the cable, and the length of the sensing aria is 3.0 mm. GOD has been immobilized by cross-linkage method using BSA and GDA, or entrapping method using an electro-polymerized polypyrrole membrane. The sensor has been dip-coated with a glucose semipermeable membrane from a solution of cellulose diacetate in acetone/ethanol. Both sensors linearly respond to glucose concentration up to 700 mg/dl within 1-3 min under 5% of oxygen tension.
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13
Impedometryによる二分子膜フィルム電極のセンサ機能
中嶋直敏・山口淑久・真鍋 修
長崎大工
IMPEDOMETRIC BILAYER FILM SENSOR
Naotoshi NAKASHIMA, Yoshihisa YAMAGUCHI and Osamu MANABE
Department of Applied Chemistry, Nagasaki University
Nagasaki 852, Japan
Potential use of bilayer film electrodes as a sensor for various gases was ezamined in terms of impedance technique. Polyion-complexed synthetic lipids was used bilayer as pattern electrode-modifying materials. Prepared bilayer electrodes did not response to hydrophobic gases; on the other hand the impedance of the electrodes changed drastically by the addition of trimethylamine, triethylamine, ethanol, acetic acid, H2O and SO2. Decrease in impedance would be caused by the formation of electroconductime carriers at the bilayer surfaces.
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14
肝細胞培養へのフォトリソグラフィー基板の応用
宮本重幸・大橋昭王・木村 純・戸辺成四郎*・赤池敏宏**
日本電気資源研・神奈川科技アカデミー*・東工大生命理工**
AN APPLICATION OF PHOTOLITHOGRAPHIC PLATES TO HEPATOCYTE CULTURE
Shigeyuki MIYAMOTO, Akio OHASHI, Jun KIMURA, Seishiro TOBE* and Toshihiro AKAIKE**
NEC Corporation, Resources & Environment Protection Research Laboratories
Kawasaki, Kanagawa 216, Japan
*Kanagawa Academy of Science and Technology
Kawasaki, Kanagawa 213, Japan
**Faculty of Bioscience and Biotechnology, Tokyo Institute of Technology
Yokohama, Kanagawa 227, Japan
Hepatocyte culture is accomplished on collagen-patterned plates prepared by means of partially collagen absorption on a quartz plate surface by photolithographic method. Adult rat hepatocytes obtained by collagen perfusion method are cultured on the patterned plate at 37℃ and hepatocytes on the plates are observed. When hepatocyte culture is carried out on a collagen patterned plate, hepatocyter are spread and adhered along the collagen absorbing regions. As the results, adhesion location of hepatocytes is controlled and hepatocyte patterning is realized.
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15
水晶ラム波デバイスを用いた免疫センサ
吉木政行・村上 徹*・宮本重幸*・大橋昭王*・栗山敏秀・木村 純*・Jukka Lekkala**
日本電気マイクロ研・日本電気資源環境技術研*・フィンランドテクニカルリサーチセンタ**
AN IMMUNOSENSOR USING A QUARTZ LAMB WAVE DEVICE
M.YOSHIKI, T.MURAKAMI*, S.MIYAMOTO*, A.OHASHI*, T.KURIYAMA, J.KIMURA* and Jukka LEKKALA**
Microelectronics Research Laboratories, NEC Corporation
Sagamihara-shi, Kanagawa 229, Japan
Resources & Environment Protection Research Laboratories, NEC Corporation
Miyamae-ku, Kawasaki-shi, Kanagawa 216, Japan
Technical Research Center of Finland
Tampere, Finland
A quartz Lamb wave device is applied to an immunosensor, where a surface mass change caused by an immunoreaction is detected as a phase shift change. Mass change amplification by latex labeled antigens is also used for high sensitive detection.
The results are followed:
(1) Mass sensitivity of an quartz Lamb wave device, which is made from a quartz wafer 80μm thick, is about 0.56 degree/(1μg/cm2) at 4.5 MHz.
(2) The adsorption amount depends on the concentration of antigen in the sample solution. Concentration from 0 μg/ml to 4 μg/ml were measured.
From these results, the Lamb wave device is useful as a immunosensor.
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16
匂い成分の定量分析における定量的脱着法の開発
松岡英明・山田善弘・銅崎慎二・根本泰行・篠原麻男*・佐藤朗好*
東農工大工・高砂香料総研*
DEVELOPMENT OF QUNATITATIVE DESORPTION SYSTEM IN QUNATITATIVE ANALYSIS OF ODOR COMPOUNDS
Hideaki MATSUOKA, Yoshihiro YAMADA, Shinji DOUSAKI, Yasuyuki NEMOTO, Asao SHINOHARA* and Akiyoshi SATOH*
Department of Biotechnology, Faculty of Technology, Tokyo University of Agriculture and Technology
2-24-16 Nakamachi, Koganei, Tokyo 184, Japan
*Central Research Laboratory, Takasago International Corporation
5-36-31 Kamata, Ota-ku, Tokyo 144, Japan
In order to develop a sensitive analyzing system for odor compounds, it is necessary to develop a quantitative adsorption-desorption system. The authors have found that Teflon particle is promising material as adsorbent applicable to such a system. The present study describes the control of desorption of odor compound from Teflon particle by controling its temperature. The Teflon particle was fully washed and packed in a glass column and used as a sampling column. Benzyl aceatate (example of odor compound) was adsorbed in the sampling column and set in a heating unit. BA desorbed from the sampling column was transferred to a cold trap in gas-chromatograph cooled at -130℃ with liquid N2. Then the cold trap was heated abruptly and BA was sent to a capillary column and analyzed. The newly developed system could control temperatures at heating unit and cold trap. Quantitative desorption of BA from Teflon particle was possible by the controling those temperatures.
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17
水晶振動子法によるモンモリロナイト薄膜の膨潤現象の解析
岡島武義・桜井英孝*・小山 昇*・徳田耕一・大坂武男
東工大総合理工・東農工大工*
STUDY ON SWELLING OF MONTMORILLONITE CLAY FILMS BY USE OF QUARTZ CRYSTAL OSCILLATORS
Takeyoshi OKAJIMA, Hidetaka SAKURAI, Noboru OYAMA, Koichi TOKUDA and Takeo OHSAKA
Department of Electronic Chemistry, Graduate School at Nagatsuta, Tokyo Institute of Technology
Midori-ku, Yokohama 227, Japan
Department of Applied Chemistry, Tokyo University of Agriculture and Technology
Koganei, Tokyo184, Japan
The piezoelectric admittance measurements of the quartz crystal oscillators with and without a montmorillonite clay coating in contact with 0.01〜1.0 M Na2SO4 aqueous media were carried out over a frequency range covering the area of the resonant frequency of each oscillator system. The results were represented in the form of conductance and susceptance spectra. By use of the conventional electrical equivalent circuit model, the relevant circuit parameters (i.e., resistance R, inductance L, and capacitance C) were evaluated as a function of the concentration of Na2SO4. The values of R obtained for the oscillator with the clay coating were found to be larger in lower Na2SO4 concentrations than in higher ones, in contrast to the case of the oscillator without the clay coating. These results were explained on the basis of the electrolyte concentration-dependent swelling of clay film as well as DLVO theory being proposed for the interaction forces between colloidal particles.
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18
テトラフェニルポルフィリンコバルト(III)錯体を感応物質とするCWEのアニオン選択性
阿部秀夫*・矢崎寛美・国府田悦男
山本製作所技研*・筑波大応生化系
ANION SELECTIVITY OF CWE BASED ON COBALT (V) TETRAPHENYLPORPHRIN COMPLEXES
Hideo ABE*, Hiromi YAZAKI and Etsuo KOKUFUTA
*Research Laboratory, Yamamoto Mfg. Co., Ltd.,
Tokorozawa, Saitama 359, Japan
Institute of Applied Biochemistry, University of Tsukuba
Tsukuba, Ibaraki 305, Japan
The coated wire electrode (CWE) was prepared using several Co(V)complexes of tetraphenylporphyrins as the carriers. The CWE exhibits a high selectivity toward such specific anions as NO2- and I-, which is clearly different from that of an electrode based on a classic anion-exchanging carrier. The selectivity of the CWE varies depending not only on the structure of the porphyrin ring, but also on the axial ligand coordinated to the central Co(V) metal.
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19
電気化学的に堆積したpH応答性RuO2薄膜の作製とその特性
パストール・カールマン・関口 敦、下 紳郎、喜多村昇、増原 宏
新技団・極微変換プロジェクト
ELECTROCHEMICALLY DEPOSITED pH-SENSITIVE RuO2 FILM
Kalman PASZTOR, Atsushi SEKIGUCHI, Nobuo SHIMO, Noboru KITAMURA and Hiroshi MASUHARA
Microphotoconversion Project, ERATO, Research Development Corporation of Japan
1280 Kami-izumi, Sodegaura, Chiba 299-02, Japan
Preparation and pH sensing properties of electrochemically deposited RuO2 films are reported. Films were deposited onto Au wires from aqueous solution of K2RuO4 by a potential cycling technique. The open-circuit potential of electrodes was linear against pH in wide range (2-12) with a slope of the least-squares regression lines between -57 and -59 mV/pH (as prepared) as well as -62 and -64 mV/pH (after 10 days). The extrapolated potential at pH=0 of the linear fitting varied between 0.421 V and 0.526 V. The pH response was stabilized after 2 days aging in distilled water. Ionic interferences were also measured in buffer solution. Among the seven kinds of adding salts, the largest positive and negative shift in electrode potential were measured in the case of MgCl2 and KI reagents, respectively. The characterized electrode was applied to measure light-induced pH increase of aqueous solution containing triphenylmethane leucohydroxide as hydroxide ion emitters and related systems.
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20
pH調整機能付アンモニアセンサの開発
伊藤雅樹・山懸 裕・金子光範*
ヤマハ発動機・エイブル*
DEVELOPMENT OF pH AJASTABLE AMMONIA SENSOR
Masaki ITO, Hiroshi YAMAGATA, Mitsunori KANEKO*
Yamaha Motor Co., Ltd
2500 Shingai Iwata, Shizuoka 438, Japan
ABLE Co., Ltd
4-15 Higashigokencho, Shinjuku-ku, Tokyo 162, Japan
pH ajastable ammonia sensor by electrolysis was investigated. In this sensor, out put was good relation between the Indole-phenol method in the very wide concentration rang from 10-1 to 10-5 mol/L. The response time of this sensor was no more than 2 minuts.
The present device would be useful one as an on line sensor from monitoring in a variety fields.
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21
多孔質Al2O3上に作成したFe2O3系薄膜センサの感湿・感ガス特性
深澤真理・松崎英樹・原 和裕
電機大工
HUMIDITY- AND GAS-SENSING PROPERTIES WITH AN Fe2O3 FILM SPUTTERED ON A POROUS Al2O3 FILM
Mari FUKAZAWA, Hideki MATSUZAKI and Kazuhiro HARA
Department of Electrical Engineering, School of Engineering, Tokyo Denki University
2-2 Knda Nishikicho Chiyoda-ku, Tokyo 101, Japan
Humidity-and gas-sensing properties with an Fe2O3 film sputtered on a Porous Al2O3 film have been investigated.
A porous Al2O3 film was formed by anodizing the deposited Al film on an Al2O3 substrate in sulphuric acid or phosphoric acid. Another thin Al2O3 film was deposited on the porous Al2O3 film with rf sputtering technique. Then an Fe2O3-based film was successively deposited on it with rf sputtering technique. Finally, Au was deposited on it as a top electrode with the substrate inclined.
The capacitance between the unanodized Al and the top electrode increased with relative humidity increased. The sensor formed at a higher anodizing voltage. While the sensor formed in sulphuric acid was sensitive to humidity for a middle humidity range, some samples formed in phosphoric acid were sensitive in a low humidity range.
All these properties have been explained by considering the distribution of the pore diameters as well as the pore shape.
The impedance of a sensor decreased at the substrate temperature of 420℃ when exposed to a H2, CO, C2H4 or I-C4H10 gas diluted in a fresh air.
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22
平面型限界電流式酸素センサの高温における感湿特性
八木秀明・堀井克彦
日本特殊陶業中研
HUMIDITY SENSING CHARACTERISTICS OF A LIMITING CURRENT TYPE PLANE OXYGEN SENSOR IN HIGH TEMPERATURE ENVIRONMENT
Hideaki YAGI and Katsuhiko HORII
Research & Development Center (NGK SPARK PLUG CO., LTD.,
2808 Iwasaki Komaki-shi, Aichi 485, Japan
A limiting current type plane oxygen sensor was developed, which being quite different from the conventional limiting current type one. The cathode of the new sensor also serves as a hole to limit gas diffusion. Studies were made to verify the humidity sensing characteristics of this sensor at temperatures over 100℃. We found that the ratio of the water vapor pressure to the IL2/IL1 (the ratio of the 2nd limiting current to the 1st limiting current) was constant. Utilizing the constancy of the ratio, now we can measure humidity accurately regardless of the sensor deterioration or the performance variation among the sensor tips.
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23
酸化マンガンを用いた湿度センサ
徐 超男・宮崎和英
福岡大工
HUMIDITY SENSOR USING OXIDES OF MANGANESE
Chaonan XU and Kazuhide MIYAZAKI
Department of Chemical Engineering, Faculty of Engineering, Fukuoka University
Fukuoka 814-01, Japan
It has been found that specific species of oxides of manganese (Mn) are sensitive to humidity (H2O) with an outstanding selectivity and a good recoverable response at room temperature. The value of electrical resistance (R) and sensitivity (S) to H2O of these sensors greatly depends on the kind of oxide of Mn employed. In the range above 50% RH, the sensors consisting of low valency oxides (Mn2O3 or Mn3O4) have shown much higher values of resistance and sensitivity to humidity, compared with the ones composed of MnO2. By means of mixing MnO2 in the sensors, R in dry environment and S vs. R characteristics have been greatly improved. As a result, humidity can be detected linearly in a wide range with sensor composed of 10 wt% MnO2 plus 90 wt% Mn3O4.
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24
複素インピーダンス法による容量型CO2センサのCO2検知機構の解明
石原達己・米谷和浩・水原由加子・滝田祐作
大分大工
STUDY ON DETECTION MECHANISMS OF CAPACITIVE TYPE CO2 SENSOR WITH COMPLEX IMPEDANCE ANALYSIS
Tatsumi ISHIHARA, Kazuhiro KOMETANI, Yukako MIZUHARA and Yusaku TAKITA
Department of Environmental Chemistry and Engineering, Faculty of Engineering, Oita University
Oita 870-11, Japan
Detection mechanisms of capacitive type CO2 sensor, CuO-BaTiO3, were studied with complex impedance analysis. From the complex impedance measurement, the equivalent circuite of CuO-BaTiO3 capacitor can be expressed by the series connection of the four parallel resistors and capacitors which correspond to the intragrain, interface between CuO and BaTiO3, electrode interface, and electrode itself. The point at the operation frequency of sensor, 50 kHz, exists on the arc corresponding to the interface between CuO and BaTiO3, and the capacitance of the interface between CuO and BaTiO3 is sensitive to CO2. Therefore, the grain interfaces between CuO and BaTiO3 is of importance for the CO2 detection on these mixed oxide capacitors. Since the energy barriers which appear at the interface between oxides depend on the semiconducting property of oxide, semiconducting property of oxide is regarded as an importance factor for deremining the CO2 sensing characteritic.
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25
ナトリウムイオン伝導性セラミックスを用いた炭酸ガスセンサ
真鍋太祐・松口正信・定岡芳彦・酒井義郎
愛媛大工
CO2 SENSING CHARACTERISTICS OF THE SOLID-STATE ELECTROCHEMICAL SENSOR BASED ON SODIUM IONIC CONDUCTOR
Taisuke MANABE, Masanobu MATSUGUCHI, Yoshihiko SADAOKA and Yoshiro SAKAI
Department of Applied Chemistry, Faculty of Engineering, Ehime University
Matsuyama-shi, Ehime 790, Japan
The sensing characteristics of a CO2 gas sensor with Na2CO3, NaHCO3 or NaOH coated on the sensing electrode were examined. Emf and response behavior for CO2 at 450℃ were independent of the coated materials, since NaHCO3 and NaOH reacted with CO2 resulting in Na2CO3. The existence of NaOH or NaHCO3 in the Na2CO3 layer induced an increase in the emf.
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26
固体電解質電極界面変化を利用したCO2センサ
日比野高士・岩原弘育
名大工
CO2 SENSOR BASED ON CHANGE OF INTERFACE STATE BETWEEN SOLID ELECTROLYTE AND ELECTRODE
Takashi HIBINO and Hiroyasu IWAHARA
Synthetic Crystal Research Laboratory, School of Engineering, Nagoya University
Furo-cho Chikusa-ku, Nagoya 464-01, Japan
The resistivity of BaCe0.95Y0.05O3-α ceramic element was very sensitive to carbon dioxide in the moisten atmosphere at high temperature. The reproducible linear relation ship between the resistivity and the CO2 concentration was observed in the range of 200 to 3000 ppm. From various electrochemical measurements, it was found that CO2 did not penetrate into the bulk of ceramic but chemisorbed on its surface and that CO2 adsorbed on the triple phase interface made the resistivity of element. Furthermore, FT-IR spectra gave information about the chemisorption of CO2 in the moisten atmosphere.
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27
炭酸塩副電極を用いた固体電解質CO2センサの応答機構
姚 勝・細原禎夫・清水陽一・三浦則雄・山添 昇
九大総合理工
SENSING MECHANISM OF SOLID ELECTROLYTE CO2 SENSOR FITTED WITH CARBONATE AUXILIARY ELECTRODE
Sheng YAO, Sachio HOSOHARA, Youichi SHIMIZU, Norio MIURA and Noboru YAMAZOE
Department of Materials Science and Technology, Graduate School of Engineering Sciences, Kyushu University
Kasuga-shi, Fukuoka 816, Japan
A sodium-ion conductor (Na3Zr2Si2PO12: NASICON)-based CO2 sensor using Li2CO3-BaCO3 electrode responded very well to CO2 in air over a wide temperature range of 350-600℃. The sensor response (electromotive force) to varying partial pressures of CO2 (PCO2)was in accordance with the 2-electron electrochemical reduction of CO2. On the other hand, the sensor response to a fixed PCO2 (2×10-3 atm) was almost independent of the partial pressure of O2(PO2) at temperatures above 450℃, while at 305℃ and below it depended on PO2 in a manner following a 2-electron reaction of O2. Thus, two types of sensing electrode reaction were indicated to occur depending on working temperature.
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28
ベタイン系色素―高分子複合膜による湿度及びNH3の検知
村田雄貴・松口正信・定岡芳彦・酒井義郎
愛媛大工
OPTICAL HUMIDITY AND NH3 GAS SENSOR USING REICHARDT'S DYE-POLYMER COMPOSITES
Yu-uki MURATA, Masanobu MATSUGUCHI, Yoshihiko SAKAOKA and Yoshiro SAKAI
Department of Applied Chemistry, Faculty of Engineering, Ehime University
Matauyama, Ehime 790, Japan
Optical intensity at 750 nm in reflection mode of Reichardt's betain dye-polymer (PMMA or PEO) composite was increased with an increase in humidity and non-actine to NH3 vapor. For the composites treated with HCl, the intensity at 590 nm was decreased with an increase in NH3 concentration of test gases and the sensitivity was accelerated by the coexistense of water vapour. Treatment with HCl induced the formation of phenolic group.
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特別講演２
次世代センサの展望
片岡照榮
シャープ東京研究所
FUTURE PROSPECTS FOR SENSOR TECHNOLOGY
Shoei KATAOKA
Sharp Corporation
273-1 Kashiwa Kashiwa-shi, Chiba 277, Japan
Future prospects for sensor technology are made from the human friendly point of view. Fundamental functions of intelligent sensors are discussed with reference to biological sensing organs. A 3D-IC character recognition sensor and an organic sensor visualizing an odor are introduced as examples of an intelligent sensor. The importance of emotion and jesture sensors is discussed for realizing a really human friendly electronic system.
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29
酸化スズ半導体を用いたNH3―選択性ガスセンサ
三橋弘和・鈴木健吾・中根正典
新コスモス電機
NH3-SELECTIVE GAS SENSOR USING TIN OXIDE SEMICONDUCTOR
Hirokazu MITSUHASHI, Kengo SUZUKI and Masanori NAKANE
New Cosmos Electric Co., Ltd
Mitsuya-Naka, Yodogawa-ku, Osaka-shi 532, Japan
An ammonia selective gas sensor was studied by using sintered tin oxide semiconductor. The addition effects of PbOx and V2O5 on the ammonia selectivity of the tin oxide semiconductor was examined. The maximum selectivity to ammonia was obtained on addition of 3 atm% PbOx and 3 atm% V2O5. In order to improved selectivity of ammonia to ethanol, WO3-Al2O3 catalyst layer was covered over the tin oxide layer. At the operation temperature of 400℃, the sensitivity to ammonia in 5 ppm was more than the sensitivity to hydrogen, ethylen and ethanol vapor in 1000 ppm. The 100% response time to ammonia in 30 ppm was less than 30 sec. The long term stability had been confirmed for 1 year.
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30
In2O3系センサ素子のオゾンガス検知特性
井樋貴夫・高尾雄二・清水康博・江頭 誠
長崎大工
OZONE SENSING PROPERTIES OF In2O3-BASED SENSORS
Takao IBI, Yuji TAKAO, Yasuhiro SHIMIZU and Makoto EGASHIRA
Department of Materials Science and Engineering, Faculty of Engineering, Nagasaki University
1-14 Bunkyo-machi, Nagasaki 852, Japan
Effects of thickness and additives on the ozone sensing properties of In2O3-based sensors have been investigated. It was revealed that the thin film type exhibited a higher O3 sensitivity than the thick film type when a pair of electrodes was located in their innermost regions, and that the surface sensitivity was superior to the interior. The surface sensitivity of a thin film In2O3 sensor was increased by doping with SnO2, especially at lower O3 concentrations, being accompanied with enlargement in surface area and resistance in air. In contrast, MgO doping resulted in a decrease in sensitivity, whereas the surface area increased. Among the sensors studied, therefore, the surface of In2O3 doped with SnO2 exhibited the highest sensitivity.
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31
Ga-doped ZnO薄膜のNO2検知特性
池田大介・松嶋茂憲・小林健吉郎・岡田元次
愛媛大工
NO2 SENSITIVE ZnO THIN FILM DOPED WITH Ga
Daisuke IKEDA, Shigenori MATSUSHIMA, Kenkichiro KOBAYASHI and Genji OKADA
Department of Applied Chemistry, Faculty of Engineering, Ehime University
Matsuyama 790, Japan
A Ga-doped ZnO thin film was deposited on a quartz substrate by RF magnetron sputtering method. The gas sensitivity of the Ga-doped ZnO film remarkably increases with decreasing the film thickness in a NO2 atmosphere. A crystallite size of the film lies in the range of 23-25 nm. Provided that all Ga atoms are ionized, a depletion-layer of the Ga-doped ZnO film is estimated to be 2 nm, being fairly smaller than the crystallite size. These results suggest that a neck between grains controls the gas sensitivity of the film to NO2.
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32
亜硝酸塩副電極を用いた固体電解質NOxセンサ
姚 勝・清水陽一・三浦則雄・山添 昇
九大総合理工
SOLID ELECTROLYTE NOX SENSOR USING SODIUM NITRITE AUXILIARY ELECTRODE
Sheng YAO, Youichi SHIMIZU, Norio MIURA and Noboru YAMAZOE
Department of Materials Science and Technology, Graduate School of Engineering Sciences, Kyushu University
Kasuga-shi, Fukuoka 816, Japan
An Na+-conductor (NASICON)-based solid electrolyte device fitted with an NaNO2 auxiliary electrode showed excellent sensing characteristics to NO and NO2 in air. The electromotive force, EMF, followed the Nernst's equation for 1-800 ppm NO and 0.1-200 ppm NO2 at temperatures of 150-240℃, the Nernst's slopes indicating one-electron reduction for both gases. In all cases, the 90% response time was in the range of 8-60 s. The increment of EMF was as large as ca. 120 mV to 100 ppb NO2 at 150℃.
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33
有機スパッタ膜を用いた全固体型マイクロ酸素センサ
大嶺政樹・内田秀和・原 正史・勝部昭明・山口秀一郎*
埼玉大工・テルモ*
SOLID STATE MICRO OXYGEN SENSOR USING SPUTTERED ORGANIC FILM
Masaki OMINE, Hidekazu UCHIDA, Masashi HARA, Teruaki KATSUBE and Shuichiro YAMAGUCHI*
Faculty of Engineering, Saitama University
Urawa, Saitama 338, Japan
*R&D Center, Terumo Co., Ltd.
Nakai-machi, Kanagawa 259-01, Japan
New type amperometric oxygen sensor was constructed by dry fabrication process. A sputtered KCl/Teflon mixed layer was applied to the ion conductive film on which Teflon film was covered as an gas permeable membrane. The Teflon film as weell as KCl/Teflon layer was prepared by a neutral ion beam sputtering. After wetting the KCl mixed layer approximately, the sensor showed a stable response to the desolved oxygen in the range 0-20 ppm.
The sensitivity and stability was strongly depended on the preparation conditions of both KCl/Teflon and Teflon layers, and the optimum sputtering conditions were investigated.
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34
TiをドープしたNb2O5の酸素センシング特性
大瀧倫卓・彭 軍・江口浩一・荒井弘通
九大総合理工
OXYGEN SENSING CHARACTERISTICS OF Ti-DOPED Nb2O5
Michitake OHTAKI, Jun PENG, Koichi EGUCHI and Hiromichi ARAI
Department of Materials S cience and Technology, Graduate School of Engineering Sciences, Kyushu University
Sensitivity of Nb2O5 as a semiconductor oxygen sensor material for air excess ratio, λ, of air-fuel mixtures is improved by doping a small amount of Ti. A nominal composition at x=0.04 of (TiO2)x(NbO2.5)1-x leads to the maximum sensitivity to oxygen in the range of x=0-0.06. At 580℃ the change of electrical conductivity between λ=0.98 and 1.02 increases from 3.88 at x=0 to 4.66 at x=0.04 in logσ. Further doping causes decrease in the sensitivity accompanying formation of Ti-rich phases. Dependence of oxygen partial pressure on electrical conductivity reveals that the extrinsic region of Nb2O5, where the conductivity changes more steeply than in the intrinsic region, considerably extends toward the lower PO2 region with Ti doping.
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35
ルテニウム錯体固定ナフィオン膜の発光消光を利用した酸素センサ
石地 徹・金子正夫*
埼玉大理工・理研*
LUMINESCENT OXYGEN SENSOR USING RUTHENIUM COMPLEX INCORPORATED IN A NAFION FILM
Toru ISHIJI and Masao KANEKO*
Saitama University, Shimoohkubo 255, Urawa-shi, Saitama 338, Japan
Permanent address: RIKEN KEIKI Co. Ltd., 2-7-6 Azusawa, Itabashi-ku, Tokyo 174, Japan
*The Institute of Physical and Chemical Research, 2-1 Hirosawa, Wako-shi, Saitama 351-01, Japan
Photoluminescent oxygen sensor is based on quenching of photoluminescence by oxygen molecule. A Nafion film incorporating ruthenium complex (Ru(bpy)32+/Nafion) was prepared by dipping the film into an aqueous solution of the complex. The emission intensity of Ru(bpy)32+/Nafion was dependent on oxygen concentration as well as on liquid medium. A good linear relationship was obtained between relative emission intensity and oxygen concentration, showing that the Ru(bpy)32+/Nafion can be used as oxygen sensor. The emission decay of Ru(bpy)32+/Nafion shows a single exponential decay in alcohol, but multicomponent decay was obtained in water and benzene. Ru(bpy)32+ is supposed to be present at boundary between hydrophobic and hydrophilic regions of the Nafion.
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36
SnO2系センサの水素ガス検知特性に及ぼすガスの拡散性と反応性の影響
中村優一郎・清水康博・江頭 誠
長崎大工
EFFECTS OF DIFFUSIVITY AND REACTIVITY OF GASES ON HYDROGEN SENSING PROPERTIES OF SnO2-BASED SENSORS
Yuichiro NAKAMURA, Yasuhiro SHIMIZU and Makoto EGASHIRA
Department of Materials Science and Engineering, Faculty of Engineering, Nagasaki University
1-14 Bunkyo-machi, Nagasaki 852, Japan
Attempts were made to clarify the effects of the diffusivity of H2 and O2 through pores and the reactivity of H2 on the sensing properties of thick film SnO2-based sensors. In the case of a pure SnO2 sensor, the surface exhibited a higher sensitivity than the interior. The addition of 1.0 wt% Pt to the sensor resulted in a drastic decrease in interior sensitivity, whereas the surface sensitivity increased slightly. Thus, it was revealed that simultaneous designing the catalytic activity and thickness of a sensor material is of primary importance in the case of the thick film sensor with a pair of electrodes in its innermost region.
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37
マイクロリング・リング電極を用いたガスセンサ
―ガスクロマトグラフィー検出器への応用―
樺澤明裕・末永智一・内田 勇
東北大工
GAS SENSING USING MICRORING・RING ELECTRODES
-APPLICATION TO A GAS CHROMATOGRAPHIC DETECTOR-
Akihiro KABASAWA, Tomokazu MATSUE and Isamu UCHIDA
Department of Molecular Chemistry & Engineering, Faculty of Engineering, Tohoku University
Aramaki-Aoba Aobaku, Sendai 980, Japan
Electrochemical behavior of microring-ring electrodes in gas phase was investigated. The electrode was prepared by deposition of carbon inside and Pt outside a grass capillary. Cyclic voltammetry at the microring-ring electrode showed that electrochemical reaction takes place at the electrode surface. Microring-ring electrode was successfully applied to a gas chromatographic detector. In the gas chromatographic experiments, the detector responded to many organic vapors. A comparison of responses demonstrated that the detector selectivity at the microring-ring electrode is somewhat different from that at an ordinary thermal conductivity detector. The detector peak increased with gas concentration of methanol.
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38
焼結酸化錫半導体ガスセンサにおける電極・半導体界面の役割
福井 清・中根正典
新コスモス電機
EFFECTS OF TIN OXIDE SEMICONDUCTOR-ELECTRODE INTERFACE ON GAS SENSITIVITY CHARACTERISTICS
Kiyoshi FUKUI and Masanori NAKANE
2-5-4 Mitsuya-Naka Yodogawa-ku, Osaka 532, Japan
The structure of gas sensor was a spherical porous tin oxide semiconductor (the 0.45 mm diameter) in which center a platinum wire coil (the 20 micron diameter) was buried. When various substances (Pt, Pd, Rh, Ag, Cu and SiO2) were previously supported on the platinum wire coil, the sensitivity characteristics changed appreciablly. The effects of the platinum was examined in detail; the platinum reduced the relative sensitivity to H2, CO and C2H5OH compared with that to CH4 and I-C4H10. At the same time, the resistance in a clean air also increased; the increase in the sensor resistance was related to a potential barrier caused by a platinum oxide formed on the platinum fine particles. The surface oxidation activity of the platinum wire coil also decreased. Thus, an important role of the potential barrier and the oxidation activity at the interface in the sensitivity characteristics was revealed.
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39
半導体式ガスセンサを用いたにおい識別システムの検討
吉田 隆・皆川良司・南条和彦・秋元靖弘・野村健次
三菱電機生活システム研
ODOR IDENTIFICATION SYSTEM USING SEMICONDUCTOR GAS SENSORS
Takashi YOSHIDA, Yoshiji MINAGAWA, Kazuhiko NANJO, Yasuhiro AKIMOTO and Kenji NOMURA
Mitsubishi Electric Corporation, Consumer Products Development Laboratory
2-14-40 Ofuna, Kamakura-city, Kanagawa 247, Japan
This paper describes how to develop odor-identifying technique by use of two different kinds of semiconductor gas-sensors and fuzzy reasoning. A combustible-gas sensor and an alcohol-gas sensor were employed, and four odor matters of fragrance, soluble coffee, cigarette smoke and ammonia were tested. The fuzzy reasoning was based on the combination of the saturated resistance from the alcohol-gas sensor and difference between the saturated resistance from the combustible-gas sensor and the other. The result of the experimental examination showed good identification degree more than 80% for the odor matters. The extended case in additional odor matters would be examined by use of this method.
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40
ガスセンサによる室内空気汚染検知と気候制御
大藪多可志・本多宗高・松浦吉展*・梶山裕久*
富山国際大・フィガロ技研*
DETECTING SYSTEM FOR AIR POLLUTION AND INDOOR CLIMATE USING TIN OXIDE GAS SENSOR
Takashi OYABU, Munetaka HONDA, Yoshinobu MATSUURA* and Hirohisa KAJIYAMA*
Department of Sociology, Toyama University of International Studies
Oyama-Cho, Toyama 930-12, Japan
*Figaro Engineering Inc.,
Minoo-shi, Osaka 562, Japan
The air purifier is a branch of air conditioning, which has been used to keep a comfortable environmental quality in domestic circumstances. Tin oxide gas sensor is used to detect the air tainted by smoke and polluted air. The sensor also has sensitivities to various gases, for example, the gases oozing from human bodies. Temperature, humidity and wind sensors are also used, and an indoor environmental quality (IEQ) is controlled simulatively by using a pulse motor fan. Comfortability is indicated as a grade by the max-min composition of fuzzy reasoning.
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