Vol. 18, Supplement A (2002)

Proceedings of the 34th Chemical Sensor Symposium
April 1-3, 2002

Abstracts

1.

Pt / WO3膜を用いた常温型水素センサの検知特性と最適化

山本菜々子、○岡崎慎司、中川英元*、朝倉祝治

横浜国大院工、東大先端研*

SENSING PROPERTIES OF A CHEMORESISTOR-TYPE HYDROGEN GAS SENSOR USING Pt / WO3 THIN FILM

Nanako YAMAMOTO, Sinji OKAZAKI, Hidemoto NAKAGAWA*, Syukuji ASAKURA

Graduate School of Engineering, Yokohama National University, Yokohama-shi, Kanagawa 240-8501, Japan
*Research Center for Advanced Science and Technology, University of Tokyo, Meguro-ku, Tokyo 153-8904, Japan

Characteristics of a chemoresistor-type hydrogen gas sensor was investigated. In the presence of hydrogen gas, impedance of Pt / WO3 thin film prepared with sol-gel method was sharply decreased at room temperature. The sensitivity depended on calcinations temperature, and exhibited the maximum around 600 deg. C. AFM observation indicated that WO3 particles in the film coagulate to form larger particles. The transient response was relatively fast even at room temperature and conductivity increased to three orders within 1 min. The high conductivity states after the hydrogen detection persisted even if the atmosphere is switched to insert nitrogen. Further the recovery rate was show and influenced by the humidity.

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2.

酸化インジウム系薄膜センサの低濃度塩素ガス検知に及ぼす酸化ランタン添加効果

○安永幸司、玉置　純、山本善史、松岡政夫

立命館大理工

EFFECT OF LANTHANUM OXIDE ON DILUTE CHLORINE GAS SENSING OF INDIUM OXIDE-BASED THIN FILM SENSORS

Koji YASUNAGA, Jun TAMAKI, Yoshifumi YAMAMOTO, Masao MATSUOKA

Department of Applied Chemistry, Faculty of Science and Engineering, Ritsumeikan University
Kusatsu-shi, Shiga 525-8577, Japan

In2O3 based thin films were prepared by suspension dropping on SiO2/Si substrate equipped with Au microelectrodes, and subjected to the detection of dilute Cl2 gas at 250 ℃. The In2O3 film showed high sensitivity to dilu te Cl2 gas in the concentration range of 0.02-5 ppm. However, the In2O3 film exhibited complicated response to Cl2 gas less than 0.05 ppm, i.e., slow response and response to opposite direction. It was found that the modification with La2O3 to In2O3 improved the sensing properties to very dilute Cl2 gas at 250 ℃. The resistance of La2O3-In2O3 sensor always incre ased upon exposure to dilute Cl2 gas. Moreover, the rate of response was much improved, i.e., the resistance reached steady state within 1 min even when the sensor exposed to dilute Cl2 gas of 0.05 ppm.

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3.

R.F.プラズマ溶射法による高感度NO2センサの製作

○史麗琴、内田秀和、勝部昭明, 尾上公正*、堀川博史*

埼玉大工，ウチヤサーモスタット*

HIGH SENSITIVE NO2 GAS SENSOR FABRICATED WITH R.F. INDUCTION PLASMA SPRAY METHOD

○Shi Liqin, H.Uchida, T.Katsube, K.Onoue*, H.Horikawa*

Faculty of Engineering, Saitama University
255 Shimo-Ohkubo, Saitama-city, Japan
*Uchiya Thermostat Co., LTD.
2-176-1 Takasu, Misato-city, Japan

This paper concerns on a high sensitive and high stable NO2 gas sensor fabricated with R.F. induction plasma spray (IPS) method. It was first shown that the IPS process is possible to provide a novel method to fabricate a gas sensitive film consisting of nanostructure particles supported by rather large particles by the control of several processing parameters of plasma spray. The resultant nanostructure SnO2 film had sufficient sensitivity to NO2 gas at the concentration less than 35 ppb with a response time less than several minutes. This technique can be applied to other gases and other materials also.

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4.

Pd/陽極酸化TiOsub>2膜センサの水素ガス検知特性とその機構

○岩永 鉄平、兵頭 健生、清水 康博、江頭　誠

長崎大工

H2 SENSING PROPERTIES AND MECHANISM OF Pd-ANODICALLY OXIDIZED TiO2 FILM

Teppei IWANAGA, Takeo HYODO, Yasuhiro SHIMIZU, Makoto EGASHIRA

Department of Materials Science and Engineering, Faculty of Engineering, Nagasaki University, 1-14 Bunkyo-machi, Nagasaki 852-8521, Japan

Nanostructured TiO2 films with sub-micron pores have been prepared by anodic oxidation of Ti plate in a H2SO4 solution at different temperatures (i.e., 5, 20 and 30°C). H2 sensing properties of these TiO2 sensors equipped with Pd and Ti electrodes were investigated at 250 and 300°C in air and N2 atmosphere. The sensor prepared at 20°C exhibited the highest H2 sensitivity in air among three kinds of the films. The sensor also exhibited reversible response to H2, and higher sensitivity in N2 than in air. XPS analysis revealed the partial formation of PdO in air, but no PdO in H2 balanced with air or N2 atmosphere. Comparison of current-voltage characteristics of the sensor between in air and in N2 confirmed higher potential barrier at Pd/TiO2 in N2 than in air. Thus, the higher H2 sensitivity in N2 is responsible for the higher potential barrier in N2, and therefore the reversible response is suggested to arise from H atoms dissociatively formed and then accumulated at the Pd/TiO2 interface.

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6.

ガスセンサ材料に応用可能な熱安定性メソポーラス SnO2 の調製

○兵頭健生，安部俊志，清水康博，江頭　誠

長崎大工

PREPARATION OF THERMALLY STABLE MESOPOROUS SnO2 FOR APPLICATION TO GAS SENSING MATERIAL

Takeo HYODO, Shunji ABE, Yasuhiro SHIMIZU and Makoto EGASHIRA

Faculty of Engineering, Nagasaki University, 1-14 Bunkyo-machi, Nagasaki 852-8521, Japan

Thermally stable mesoporous SnO2 (m-SnO2) was prepared from sodium stannate by utilizing the self-assembly of n-cetylpyridinium chloride (C16PyCl), followed by treatment with phosphoric acid (PA). The specific surface area of m-SnO2 increased with decreasing the C16PyCl concentration in the precursor solution. The secondary particle size of m-SnO2 showed the maximum value at the C16PyCl concentration of 2.0〜3.0 wt%. Among the specimens obtained, m-SnO2 prepared at the C16PyCl concentration of 0.5〜1.0 wt%, having uniform and small secondary particle (0.5〜1.0 mm by SEM) seemed to be promising as a semiconductor gas sensor material. Moreover, attempts were made to prepare a new sensor material by surface modification of conventional SnO2 powder, which was prepared by calcination of tin oxalate at 900℃ for 5 h, with m-SnO2.

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7.

半導体ガスセンサを検出器に用いたガスクロマトグラフ方式による微量ガスの定量的検知
香田弘史、花田真理子、○柳谷順子、寄吉典子、田中克之

エフアイエス

Highly Sensitive and Quantitative Analysis of Volatile Sulfer Compounds Using a Highly Sensitive Semiconductor Detector Adopted in GLC System

Hiroshi KODA, Mariko HANADA, Junko YANAGITANI, Noriko KIYOSHI, Katsuyuki TANAKA

FiS Inc.
3-36-3 Kitazono, Itami, Hyogo 664-0891, Japan

It has been demanded to detect very low concentration of volatile sulfer compounds (VSC) in odors. For this purpose, we have developed a chromatographic gas analyzer using a high sensitive indium oxide gas sensor as a detector. We have designed a small column and used environmental air as carrier gas instead of highly pressurized gas. This analyzer is small, easy-operational, and portable. This analyzer can measure the concentration of each component in the gas mixture, and quantify the concentration of VSC at lower than 1ppm. We have applied this technology in a breath analyzer.

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8.

ZnO厚膜型センサの口臭測定器への応用

○鈴木健吾、鷲尾純平*、岩倉政城*

新コスモス電機株式会社・東北大学歯学部*

APPLICATIONS OF ZnO THICK FILM TYPE GAS SENSOR IN MOUTH AIR MONITORING

Kengo Suzuki, Junpei Washio and Masaki Iwakura

New cosmos electric Co., Ltd.
Osaka, 532-0036, Japan
Department of Dentistry, Tohoku University
Sendai, 980-8575, Japan

A mouth air monitor for the diagnoses of halitosis in dental clinics has been developed, which can detect VSC selectively at concentration of lower than 1ppm in mouth air. A semiconductor type VSC sensor based on ZnO thick film and a special filter were used in the monitor, and the monitor could be worked with higher sensitivity and reliability as compared to commercialized monitors. The monitor can be used in routine chair-side study and filed surveys of halitosis with small size and simple operation.

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9

ニオイセンサによる口臭検知といやしロボットへの応用

○新保 達也、大薮 多可志、瀬戸 就一、蔡　奎千、中野 康英

金沢星稜大、金沢星陵大、金城大、新コスモス電機、三協アルミ

Detection of Breath Odor Using Metal Oxide Gas Sensors and Its Application to Welfare Fields

Tatsuya SHINBO, Takashi OYABU, Shuichi SETO, Kuiqian CAI, Yasuhide NAKANO

Kanazawa Seiryo University, Kanazawa 920-8620, Japan
Kinjo College, Matto 924-8511, Japan
New Cosmos Electric Co.LTD., Osaka 532-0036, Japan
Sankyo Aluminium Industry Co.LTD., Takaoka 933-0957, Japan

Three types of metal oxide gas sensors were adopted to detect the degree of breath odor. Various sorts of information are included in the odor. Each sensor has different sensitivities to gaseous chemical substances and the sensitivities also differ according to human behaviors, for example taking a meal, teeth-brushing and drinking something. There is also a possibility that the sensor can detect degrees of daily fatigue. Sensor sensitivities were low for the expiration of the elderly when the subject drank green tea. In this study, it is thought that the odor system can be incorporated into a healing robot. The robot can communicate with the elderly using several words and also connect to Internet. As for the results, the robot can identify basic human behaviors and recognize the living conditions of the resident. Moreover, it can also execute a kind of information retrieval through the Internet. Therefore, it has healing capability for the aged, and can also receive and transmit information.

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特別講演

時間応答を生かす能動型知的センサ

◯吉川 研一

京都大学大学院理学研究科

INTELLIGENT SMELLING MACHINE WITH NONLINEAR DYNAMIC RESPONSE

Kenichi YOSHIKAWA

Department of Physics, Graduate School of Science, Kyoto University Kyoto, 606-8502, Japan

A novel gas sensing system based on the information embedded in a nonlinear dynamic response is proposed. By applying a sinusoidal voltage to a heater attached to SnO2, characteristic time-dependent response of the sensor resistance is obtained for environmental gases. In order to evaluate the nonlinear time-dependent response in a quantitative manner, Fast Fourier Transform (FFT) is performed for the dynamic response. Higher harmonics, obtained by performing the FFT, were processed using suitable numerical methods. In the actual experiments, it is shown that eight different gases (methanol, ethanol, acetone, diethyl ether, iso-butane, benzene, ammonia and ethylene) as well as natural air can be identified and also quantitated with a single detector.

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受賞講演

セラミックスの微細組織制御によるガスセンシング機能の向上とそのメカニズム の解明

兵頭健生

長崎大工

MECHANISM OF SENSITIVITY ENHANCEMENT OF SEMICONDUCTOR GAS SENSORS INDUCED BY MICROSTRUCTURAL CONTROL

Takeo HYODO

Faculty of Engineering, Nagasaki University
1-14 Bunkyo-machi, Nagasaki 852-8521, Japan

Control of nano- and meso-structures of semiconductor oxides is of primaly importance in order to get high performance gas sensors. In the paper, two techniques are introduced among our current researches directed to evaluating and controlling the microstructure of semiconductor oxides. (1) A.c. impedance measurement was performed to investigate the variation in potential barrier height per grain boundary. The change in the potential barrier height induced by gas was found to be the most important factor in determining the gas-sensing properties of various varistor-type gas sensors (diethoxydimethylsilane-modified SnO2, Bi2O3-Nb2O5 and ZnO-based oxides and so on). (2) Ordered mesoporous SnO2 powders were prepared from sodium stannate by utilizing the self-assembly of n-cetylpyridinium chloride, followed by treatment with phosphoric acid. The treatment was indispensable for maintaining the mesoporous structure of SnO2 up to 700ーC.

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10.

拡散方程式に基づく薄膜型半導体ガスセンサの解析-回復時における膜内からのガス の消失挙動-

○松永直樹、酒井　剛、島ノ江憲剛、山添　f

九大院総理工

DIFFUSION EQUATION-BASED STUDY OF THIN FILM SEMICONDUCTOR GAS SENSOR - GAS VANISHING BEHAVIOR IN SENSING FILM AT RECOVERY STAGE -

Naoki MATSUNAGA, Go SAKAI*, Kengo SHIMANOE*, Noboru YAMAZOE*

Department of Molecular and Materials Sciences, Graduate School of Engineering Sciences,
*Department of Molecular and Materials Sciences, Faculty of Engineering Sciences, Kyushu University
Kasuga-shi, Fukuoka 816-8580, Japan

A diffusion-reaction equation was solved under non-steady condition in order to simulate how the target gas inside a sensing film would vanish after the flow of the target gas over the film is switched off suddenly. The solution was expressed by a polynomial function involving diffusion coefficient (D), rate constant (k), film thickness (L), depth from the film surface (x), time (t) and initial target gas concentration outside (Cs). Concentration profiles of the target gas in the film at various time periods after the switching off were simulated for the two cases of k = 108 and 0 sec-1. It was shown that the time period needed for the gas to vanish out (recovery time) is given approximately by L2/D for k = 0, while it becomes shorter somewhat for larger values of k. It was pointed out that the response and recovery times of actual sensors, much longer than simulated here based on the diffusion equation, should be dominated by the surface process of the individual grains of metal oxide used.

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11.

電界効果トランジスタNO2センサにおける妨害ガスの検討

○中田聖士、島ノ江憲剛、三浦則雄*、山添　f

九大院総理工,*九大先端センター

EFFECT OF COEXISTENT GASES ON FET NO2 SENSOR ATTACHED WITH NaNO2-BASED AUXILIARY PHASE

Seiji NAKATA, Kengo SHIMANOE*, Norio MIURA**, Noboru YAMAZOE*

Department of Molecular and Materials Sciences, Graduate School of Engineering Sciences, Kyushu University
*Department of Materials Science, Faculity of Engineering Sceiences, Kyushu University
**Advanced Science and Technology Center for Cooperative Research, Kyushu University
Kasuga-shi, Fukuoka 816-8580, Japan

The NO2 sensor for which an FET chip was combined with a NaNO2-WO3 auxiliary phase was tested for the stability of its sensing signal to dilute NO2 in the presence of CO2, NO or water vapor at 130℃. It was found that CO2 is totally unharmful, allowing the sensor to detect as low as 10 ppb NO2. On the other hand, NO was found to be an active gas responded by the sensor, although its sensitivity is one tenth the NO2 sensitivity so that it would remain unharmful under its concentration exceeds 100 ppb. Finally, water vapor was found to cause the base line of signal output to shift downward significantly. The effect could be reduced drastically with a rise in firing temperature of the gold electrode used.

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12.

Pt／WO3／SiC構造ダイオードの電気的特性の雰囲気ガスによる変化

○中込　真二、奥田　浩二、國分　義弘

石巻専修大理工

CHANGE OF THE ELECTRICAL PROPERTIES OF Pt／WO3／SiC STRUCTURE DIODE DEPENDING ON THE AMBIENT GAS

Shinji NAKAGOMI, Kouji OKUDA and Yoshihiro KOKUBUN

Department of Information Technology and Electronics, School of Science and Engineering, Ishinomaki Senshu University, Ishinomaki-shi, 986-8580, Japan

The diode based on silicon carbide with Pt-thin WO3 layer-SiC structure was fabricated. The current-voltage and capacitance-voltage characteristics were measured in H2 and O2 ambient in range from 25 to 300℃. The series resistance of the diode in O2 ambient was increased with an increase in the thickness of WO3. This brought about an increase in the voltage response up to 3 volts depending on the forward current. The slope of 1／C2-V plot of the diode became gentle with increasing temperature in H2 ambient and became gentle in higher H2 concentration at 300℃. The effective area of electrode evaluated from the slope depends on the ambient H2 concentration.

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13.

薄膜複合光導波路を用いる超高感度アンモニアセンサ

◯アブリズ イミテ、伊藤公紀、村林真行


横浜国立大学院

AN EXTREMELY HIGH SENSITIVE AMMONIA SENSOR BASED ON THIN FILM COMPOSITE OPTICAL WAVEGUIDE

◯ Abliz YIMIT**, Kiminori ITOH*, Masayuki MURABAYSHI*

Graduate School of Environment and Information Sciences, Yokohama National University
Tokiwadai, Hodogaya ku, Yokohama 240-8501, Japan
*Department of Chemistry, Xinjiang University, Urumqi, 830046, China

An optical waveguide sensor with a thin film composite structure is fabricated and its application in sensing extremely low concentration of ammonia has been demonstrated. The highly sensitive element are based on (1) a bromothymol blue (BTB) film/potassium ion exchanged (PIE) glass composite optical waveguide (COWG), (2) polytungstic acid (PTA) film/PIE glass COWG and (3) TiO2 film/PIE glass COWG coated with a pure BTB film onto the PTA and TiO2 surface. In the presence of ammonia, the BTB film changes color from yellow to blue, which causes absorption of the 633nm guided wave. The sensor has a short response time and a high sensitivity. The BTB/PIE and PTA /PIE glass COWG has a detection limit of 1ppb ammonia. We also used a highly sensitive TiO2 film/PIE glass COWG which detected 1ppt ammonia.

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14.

プラズマ重合分子認識膜を有するQCMガスセンサ

○真田尚治，信山健次，草野英二，金原　粲，南戸秀仁，松本高利*，黒澤　茂*，田辺和俊*，大藪多可志**

産業技術総合研究所*，金沢経済大学**

QCM GAS SENSOR WITH PLASMA-POLYMERIZED MOLECULAR RECOGNITION-FILM

Syouji SANADA, Kenji NOBUYAMA, Eiji KUSANO, Akira KINBARA, Hidehito NANTO, Takatoshi MATSUMOTO*, Shigeru KUROSAWA*, Kazutoshi TANABE*, Takashi OYABU**

Adv. Mat. Sci. R&D Center, Kanazawa Inst. of Tech.
3-1 Tatsukaho Matto-shi, Ishikawa 924-0838, Japan
*National Inst. of AIST
**Kanazawa University of Economics

Quartz crystal microbalance (QCM) gas sensors coated with films of styrene, acrylic acid or methacrylic acid, etc. as the molecular recognition membrane are prepared using plasma-polymerized CVD method. The sensor coated with acrylic acid or methacrylic acid film exhibits an excellent selectivity and a high sensitivity for ammonia gas. On the other hand, the sensor coated with styrene film responded to various gases. These sensors are useful in a sensor array in conjunction with pattern recognition analysis for identification of gases and odors.

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15.

NASICONを用いた室温作動型CO2センサにおける水蒸気の役割

○小畑賢次、島ノ江憲剛、三浦則雄*、山添　f

九大院総理工、九大先端センター*

INFLUENCES OF WATER VAPOR ON NASICON BASED CO2 SENSOR OPERATIVE AT ROOM TEMPERATURE

Kenji OBATA, Kengo SHIMANOE*, Norio MIURA** and Noboru YAMAZOE*

Department of Molecular and Material Sciences, Interdisciplinary Graduate School of Engineering Sciences, Kyushu University
*Department of Materials Science, Faculty of Engineering Sciences, Kyushu University
**Advanced Science and Technology Center for Cooperative Research, Kyushu University, Kasuga-shi, Fukuoka 816-8580, Japan

The NASICON (Na3Zr2Si2PO12)-based CO2 sensor operative at room temperature is shown to be deeply influenced by water vapor in three ways. First, water vapor promotes spontaneous formation of NaHCO3 and/or Na2CO3 as an auxiliary phase by soaking Na3PO4 impurity out of the NASICON disk even when no auxiliary phase is introduced externally. Second, water vapor participates in the CO2-sensing electrode reaction, probably in the form of chemisorbed water on the oxide electrode (In2O3) used. Third, the EMF vs. CO2 concentration correlation (or base EMF) shifts up with increasing humidity, accompanied by a decrease in the impedance of the sensing electrode.

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16.

NASICON膜を用いたプレーナ型CO2センサ　−膜構造とセンサ特性−

○宮地祐治、木田徹也、酒井　剛、島ノ江憲剛、山添　f

九大院総合理工

PLANAR TYPE CO2 SENSOR USING NASICON THICK FILM - FILM STRUCTURE AND SENSING PROPERTY-

Yuji MIYACHI, Tetuya KIDA, Go SAKAI*, Kengo SHIMANOE*, Noboru YAMAZOE*

Department of Molecular and Material Sciences, Interdisciplinary Graduate School of Engineering Sciences, Kyushu University
Kasuga-shi, Fukuoka 816-8580, Japan
*Department of Materials Science, Faculty of Engineering Sciences, Kyushu University
Kasuga-shi, Fukuoka 816-8580, Japan

Densification of thick films of NASICON (Na+ conductor, Na3Zr2Si2PO12) was explored for the use in a planar CO2 sensor. Among the many kinds of dispersants of NASICON powder for the screen printing tested, ethylene glycol was found to exhibit the best densified NASICON thick film after calcination at 1000℃, together with good adhesion to the alumina substrate and good mechanical strength. As observed on SEM, the NASICON thick film fabricated from the ethylene glycol paste obviously showed much improved surface morphology compared with that from a conventional dispersant (α-terpineol + ethyl cellulose). Owing to the densification of the film, the resulting planar type CO2 sensor device attached with a binary carbonate auxiliary phase (Li2CO3-BaCO3) showed good CO2 sensing properties at 400-450℃ under humid as well as dry conditions.

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17.

高温でのトータルNOxの検出が可能な複素インピーダンス応答型ジルコニアセンサ

三浦則雄、○中藤充伸、セージ・ズイコフ

九大先端センター

IMPEDANCE-BASED SENSOR USING STABILIZED ZIRCONIA FOR SENSING TOTAL NOx AT HIGH TEMPERATURE

Norio MIURA, Mitsunobu NAKATOU, Serge Zhuiykov

Advanced Science and Technology Center for Cooperative Research, Kyushu University, Kasuga-shi, Fukuoka 816-8580, Japan

We report here a new-type zirconia-based sensor that can detect total NOx content at high temperature such as 700℃. A closed-one-end yttria-stabilized zirconia (YSZ) tube was used as a base sensor material. An oxide sensing electrode (SE) and a Pt counter electrode (CE) were formed on the outer and inner surfaces of the YSZ tube, respectively. The complex impedance of the device using a ZnCr2O4-sensing electrode was measured with an impedance analyzer in the frequency and the temperature ranges 0.1 Hz-100 kHz and 600-700℃, respectively. A large semicircular arc was observed in complex impedance plots (Cole-Cole plots) in the lower frequency range examined and it seemed to correspond to the electrolyte/electrode interface. The impedance value at 1 Hz of the present device was found to vary almost linearly with the concentration of NO (or NO2) from 50 to 400 ppm in the sample gas at 600-700℃. Furthermore, it is noted that the sensitivity of NO is almost equal to that of NO2. This means that the present device can detect the total NOx at higher temperatures.

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18.

希土類のオキシ硝酸塩を検出極に用いた新規な固体電解質型NOガスセンサ

○小田篤、田村真治、今中信人、足立吟也

阪大院工

A NEW SOLID ELECTROLYTE TYPE NITROGEN MONOXIDE GAS SENSOR WITH THE RARE EARTH OXYNITRATE BASED AUXILIARY ELECTRODE

Atsushi ODA, Shinji TAMURA, Nobuhito IMANAKA, Gin-ya ADACHI

Materials Chemistry, Division for Research of Engineering Osaka University 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan

A new solid electrolyte type nitrogen monoxide (NO) gas sensor was fabricated by using multivalent cation and divalent oxide anion conducting solid electrolytes with the rare earth oxynitrate based auxiliary electrode. The linear relationship between the sensor output and the NO content was obtained in the range from 200 to 2000 ppm, and the n value calculated from the EMF slope is 0.91 for the sensor with EuONO3+KNO2 as the auxiliary electrode. A quantitative NO gas detection was successfully realized with a rapid, stable, continuous, and reproducible response. The present NO gas sensor is greatly expected to be applied at various NO gas exhausting sites.

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19.

塩化物イオンおよび３価イオン伝導体を組み合わせた新規な塩素ガスセンサ

○田村真治、岡本浩治、今中信人、足立吟也

阪大院工

A NEW TYPE OF Cl2 GAS SENSOR WITH Cl- AND Al3+ ION CONDUCTING SOLID ELECTROLYTES

Shinji TAMURA, Koji OKAMOTO, Nobuhito IMANAKA, Gin-ya ADACHI

Department of Applied Chemistry, Faculty of Engineering, Osaka University
2-1 Yamadaoka, Suita, Osaka 565-0871, Japan


A compact Cl2 gas sensor was fabricated with the combination of the Ca doped LaOCl solid solution prepared by a ball milling method and the Al3+ ion conducting solid electrolyte. Since La0.8Ca0.2OCl0.8 shows the extraordinary high Cl- conductivity which is ca. 2000 times higher than that of LaOCl, and the high durability even in a water vapor existing atmosphere, the present chlorine gas sensor exhibited the high sensing performance such as rapid, reproducible, and high selective response for Cl2 gas detection. In addition, an exact 1:1 relationship was achieved between the sensor output and the logarithm of the chlorine gas content and the relation exactly obeys the Nernst theoretical equation.

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20.

Ni添加LaGaO3を電解質とした電流検出型炭化水素センサ

○石原達己、福山麻都架、西口宏泰、滝田祐作

大分大工

AMPEROMETRIC HYDROCARBON SENSOR USING Ni DOPED LaGaO3 BASED ELECTROLYTE

Tatsumi ISHIHARA, Madoka FUKUYAMA, Hiroyasu NISHIGUCHI, and Yusaku TAKITA

Department of Applied Chemistry, Faculty of Engineering, Oita University, Dannoharu 700, Oita 870-1192, Japan

Amperometric hydrocarbon sensor using Ni doped LaGaO3 based oxide was investigated and it was found that the current of the sensor using Ni doped LaGaO3, Pt, and La0.6Sr0.4CoO3 for electrolyte, active, and inactive electrode is highly selective to C3H6 and hardly depend on O2 , CO, and CO2 concentration. Therefore, this sensor is highly promising as the sensor for monitoring hydrocarbon concentration in the exhaust gas. The current of the sensor is independent of thickness of electrolyte and the flow rate of sensing gas.

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21.

固体電解質を用いた改質ガス中のCOセンシング:(T) 燃料電池型センサ

○橋本衷子、浅野和代、日比野高士、佐野　充

産総研セラミックス、名大院環境

DETECTION OF CO IN REFORMED GASES USING SOLID ELECTROLYTES: (T) FUEL-CELL TYPE SENSOR

Atsuko HASHIMOTO, Kazuyo ASANO, Takashi HIBINO, and Mitsuru SANO

Ceramics Research Institute, National Institute of Advanced Industrial Science and Technology
Moriyama-ku, Nagoya 463-8560, Japan
Graduate School of Environmental Studies, Nagoya University
Chikusa-ku, Nagoya 466-0804, Japan

A Pd anode in a fuel-cell type sensor using 20 mol% Sm3+-doped ceria as the electrolyte was subject to a large and reversible change in the anodic-reaction resistance with the CO concentration in a flowing mixture of 0 - 4000 ppm CO, 50 % H2, 10 % CO2 and 6 % H2O vapor between 300 and 400 ℃. This behavior brought about an almost linear relationship between the electromotive force(EMF) generated from the cell or the short-circuit current through the cell and the logarithm of CO concentration. In both signals, the minimum detectable CO concentration was 50 ppm, and the 90 % response and 90 % recovery times were about 60 seconds. Furthermore, an improvement in the reproducibility and sensitivity of the sensor could be achieved by using 25 mol% Y3+ doped BaCeO3 with higher ion conduction as the electrolyte.
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22.

パルス式電解排出を利用した起電力型高温水素センサ

○片平幸司、岩元孝史、松本広重*、岩原弘育**

株式会社TYK、名大理工総研*、名大名誉**

HIGH TEMPERATURE GALVANIC CELL TYPE HYDROGEN SENSOR WITH PULSE-TYPE ELECTROCHEMICAL EVACUATION

Koji KATAHIRA, Takashi IWAMOTO, Hiroshige MATSUMOTO and Hiroyasu IWAHARA

TYK Corporation, Advanced Materials Research & Development Center, 3-1, Ohbata-cho, Tajimi, 507-8607, Japan
*Center for Integrated Research in Science and Engineering, Nagoya University
Furo-cho, Chikusa-ku, Nagoya, 464-8603, Japan
**The professor emeritus of Nagoya University
Furo-cho, Chikusa-ku, Nagoya, 464-8603, Japan

Galvanic cell type high temperature hydrogen sensor with pulse-type electrochemical evacuation was constructed using a proton conducting CaZr0.9In0.1O3-a ceramic as a solid electrolyte. The sensor consists of one-end-closed electrolyte with Pt electrodes inside and outside of the tube; the tube is glass-sealed to make the closed standard electrode compartment. Pulse currents determine the hydrogen activity in the standard compartment by evacuating hydrogen through the electrolyte. Ambient hydrogen activity is a function of the EMFs measured during off-current time. The plots of the EMFs against the logarithm of hydrogen partial pressure were linear with the slops which showed good coincidence with the one calculated from Nernst equation between 700 and 1000oC.

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23.

LiBr-KBrO3系電解質を用いたフッ化水素センサの反応解析

岩倉千秋、井上博史、古川直治、野原愼士、○生駒　啓，格清敏男*、堀内雅司*、石川　博*

阪府大院工，新コスモス電機（株）*

REACTION ANALYSIS OF HYDROGEN FLUORIDE GAS SENSOR USING LiBr - KBrO3 AS AN ELECTROLYTE

Chiaki IWAKURA , Hiroshi INOUE , Naoji FURUKAWA , Shinji NOHARA , Kei IKOMA, Toshio KAKUSE*, Masashi HORIUCHI*, Hiroshi ISHIKAWA*

Department of Applied Chemistry, Graduate School of Engineering, Osaka Prefecture University
Sakai, Osaka 599-8531, Japan
*NEW COSMOS ELECTRIC CO. , LTD
Osaka, Osaka 532-0036, Japan

Potentiostatic reduction of Br2 generated in LiBr + KBrO3 solution containing HF was studied to optimize and characterize the electrochemical gas sensor for monitoring HF. A linear relationship was found between the reduction current of Br2 at platinized platinum electrode and the concentration of HF in the range of 10-5 ~ 1 M at 25 ℃. Other factors such as pH, concentrations of the electrolyte, agitation affecting the Br2 reduction were examined by electrochemical and spectroscopic analyses.

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24.

水素結合性イオノフォアによる油水界面アニオン促進移動解析

○西沢精一，横堀倫之，加藤　亮，寺前紀夫

東北大院理

FACILITATED TRANSFER OF ANIONS ACROSS THE LIQUID/LIQUID INTERFACE BY HYDROGEN-BONDING IONOPHORES

Seiichi NISHIZAWA, Tomoyuki YOKOBORI, Ryo KATO, Norio TERAMAE

Department of Chemistry, Graduate School of Sience, Tohoku University
Aoba-ku, Sendai 980-8578, Japan

Dihydrogenphosphate transfer across the nitrobenzen (NB)/water interface facilitated by hydrogen-bonding ionophores 1 to 3 is studied by using ion transfer polarography. While mono-thiourea 3 cannot effectively facilitate the transfer of H2PO4-, bis-thiourea 2 has a significant ability to facilitate H2PO4- transfer across the NB/water interface. Remarkably, the analysis of ion transfer polarograms shows that the H2PO4- transfer is assisted by 1:2 complexation between 2 and H2PO4-. The formation of a 1:2 complex in the NB phase is also supported by 1H NMR spectroscopy. Despite the apparently identical binding mode based on two point hydrogen-bonding interactions, the H2PO4- transfer with bis-thiourea 2 is indeed stabilized by more than 12 kJ mol-1 as compared to the case with mono-thiourea 3. Furthermore, the stabilization of the H2PO4- transfer obtained for bis-thiourea 2 is even larger by 10.6 kJ mol-1 than the stabilization obtained for highly preorganized bis-thiourea 1, in which four hydrogen bonds are involved in the formation of a 1:1 complex with H2PO4-. The results in the present work suggest that use of relatively flexible ionophores like bis-thiourea 2 may be suited for the design of ionophore-based chemical sensors for H2PO4-.

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25.

ヘテロコア型光ファイバを用いる屈折率の測定

○関　篤志、伊賀光博、平間恭子、平成明朝中澤　毅、田辺弘幸、渡辺一弘

創価大工

MEASUREMENT OF REFRCTIVE INDEX USING HETERO-CORE TYPE FIBER OPTIC

Atsushi SEKI, Mitsuhiro IGA*, Kyoko HIRAMA*, Tsuyoshi NAKAZAWA*, Hiroyuki TANABE, Kazuhiro WATANABE*

Department of Bioenginnering, *Department of Information systems, Faculty of Engineering, Soka University
1-236 Tangi, Hachioji, Tokyo 192-8577, Japan

New_YorkRefractive indices sensor based on hetero-core fiber optic was fabricated by preparing silver film on hetero-core portion of the fiber. Transmission loss of the propagating light was taken place by resonance of evanescent wave at the cladding/silver interface and surface plasmon at the silver film. The loss increased with being subjected to depositing of silver film on the fiber surface. The loss increased according to the increasing of refractive indices of the outer environment. In sucrose solution, the plots of ΔNew_Yorkloss versus concentration were linear in the range of 0 ミ 30 %. Furthermore, refractive indices change was observed when self-assembly monolayer of alkane thiol was formed on the silver surface.

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26.

弾性表面波センサを用いた液体フロー系計測システムの開発

○近藤 淳，松井義和，塩川祥子

静大工

DEVELOPMENT OF LIQUID-FLOW SENSING SYSTEM WITH SURFACE ACOUSTIC WAVE SENSOR

Jun Kondoh, Yoshikazu MATSUI, Showko SHIOKAWA

Department of Systems Engineering, Faculty of Engineering, Shizuoka University, Hamamatsu-shi, Shizuoka 432-8561, Japan

A liquid-flow system with shear horizontal surface acoustic wave (SH-SAW) sensor is developed to identify electrolytes without selective coatings. When electrical properties of samples are equal, steady-state responses from the SH-SAW sensor are the same. It is impossible to distinguish the differences of sample by only steady-state values. The transient responses from the liquid-flow system, however, depend on materials contained in the sample solution. It is possible to know information of the solution from transient responses such as ion species in it. To identify and evaluate the sample solutions, the self-calibrating ratiometric method (SCRM) is proposed. The transient responses are influenced by the experimental conditions. However, as the SCRM is based on the time differences between rise and fall and also the ratio of the output value in transient responses, the influences of experimental condition can be calibrated and so ignored. Based on the SCRM and an artificial neural network, the electrolytes are identified.

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27.

ppbレベルの2-ヒドロキシビフェニルの高感度検知が可能な再生型SPR免疫センサ

○カウベリ　ゴビ、佐々木　誠、三浦 則雄

九大先端センター

REGENERABLE SURFACE PLASMON RESONANCE (SPR)-BASED IMMUNOSENSOR FOR SELECTIVE AND SENSITIVE DETECTION OF 2-HYDROXYBIPHENYL OF PPB LEVELS

〇K. V. GOBI, Makoto SASAKI, Norio MIURA

Research Institute, National Rehabilitation Center for the Disabled
Advanced Science and Technology Center for Cooperative Research, Kyushu University Kasuga, Fukuoka 816-8580 , Japan

A highly sensitive, renewable SPR-based immunosensor for the detection of 2-hydroxybiphenyl (HBP) was developed using a model HBP-hapten compound, HBP-bovine serum albumin conjugate (HBP-BSA), and an anti-HBP-BSA monoclonal antibody. HBP-BSA conjugate was immobilized on a thin Au-film sensor chip by simple physical adsorption. Anti-HBP-BSA antibody on contact with the HBP-BSA conjugate immobilized sensor chip causes an increase in the SPR angle of the sensor chip. The immunoreaction between the immobilized HBP-BSA conjugate and anti-HBP-BSA monoclonal antibody, which could be inhibited by the presence of HBP, was followed to measure the concentration of HBP; a highly selective detection of HBP in the concentration range of 0.1 - 1000 ppb was achieved with a response time of ca. 20 min. The antibody associated with the sensor chip by antigen-antibody binding was found to be removed on treatment with a pepsin solution for few minutes. The SPR sensor chip was found to be reusable for more than 10 times without a significant decrease in the sensor response.

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28.

携帯型SPR免疫センサの作製と高感度化

○鈴木正康，北本和久，松島功治

富山大工

DEVELOPMENT OF A SPR IMMUNOSENSOR AND IMPROVEMENT OF ITS SENSITIVITY

Masayasu SUZUKI, Kazuhisa KITAMOTO, Koji MATSUSHIMA

Department of Electric and Electronic Engineering, Faculty of Engineering, Toyama University
Toyama-shi, Toyama 930-8555, Japan

The miniature and portable immunosensor system was developed by using a miniature SPR sensor chip and a non-pumping flow system. As a model case of smaller molecule measurement, 2,4-dinitrophenol (DNP) sensor was developed. DNP in the sample and the fixed number of labeled DNP were competitively bound to the anti-DNP antibody onto the sensor surface. As label compounds, bovine serum albumin, gamma-globulin and hemocyanin were compared and the largest response was obtained by using DNP-hemocyanin. In order to realize a portable immunosensor system, a non-pumping flow system was developed. By utilizing hydrostatic pressure, a simple flow system was constructed and applied to miniature SPR immunosensor measurement. The same performance was realized with this flow system as a conventional flow system using a syringe pump.

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29.

エバネセント波蛍光測定法による標的オリゴヌクレオチドのバイオセンシング

○篠原寛明、岡本康孝、宍戸昌彦

岡山大工

BIOSENSING FOR THE TARGET OLIGONUCLEOTIDE BY FLUORESCENCE MEASUREMENT WITH EVANESCENT WAVE

Hiroaki SHINOHARA, Yasutaka OKAMOTO, Masahiko SISIDO

Department of Bioscience and Biotechnology, Faculty of Engineering, Okayama University, 3-1-1 Tsushima-naka, Okayama 700-8530, Japan

Fluorescence measurement using evanescent wave excitation was applied to perform high sensitive and convenient bioaffinity sensing for the target oligonucleotide. In this paper, detection of the oligonucleotide as a model of a flagment of the p53 gene, a tumer suppressor gene, was performed at the concentration range from 10-8 to 10-6 M by using competitive hybridization reaction of the the Cy5-labeled and the non-labeled target oligonucleotides to the complimentary oligonucleotide probe immobilized on the optical waveguide. Convenient detection of the single-base mismatches of the target oligonucleotide was also demonstrated.

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30.

SPRセンサによる金黒の評価

○柘植将示*、武居修*、宇佐美論*、掘越弘毅*、加藤誠志、外山滋

国立リハビリ研、東洋大工*

EVALUATION OF GOLD-BLACK USING AN SPR SENSOR

Masashi TSUGE*, Osamu TAKEI*, Ron USAMI*, Koki HORIKOSHI*, Seishi KATO, Shigeru TOYAMA

Research Institute, National Rehabilitation Center for the Disabled
4-1 Namiki, Tokorozawa, Saitama 359-8855, Japan
*Department of Applied Chemistry, Faculty of Engineering, Toyo University
2100 Nakanodai, Kujirai, Kawagoe, Saitama 350-8585, Japan

Gold-black was electrochemically deposited on a Au-coated glass plate, and its growth was evaluated with an SPR sensor. It was found that the gold-black exhibited an extraordinary high resonance angle. We hypothesized a five-layer model, which consists of glass, Cr, Au, Au-black, and water layers, to explain the resonance angle of the gold-black plate. By assuming the refractive index of gold-black layer equal to that of the mixture of gold and water, the high resonance angle was reproduced.

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31.

酵母固定化ＳＰＶデバイスを用いた酒造用米麹の評価

○千代智之，松井圭三，村上裕二*，横山憲二*，民谷栄一*

福光屋，*北陸先端科技大

YEAST-IMMOBILIZED SPV DEVICE FOR THE ESTIMATION OF QUALITY OF RICE KOJI

T. Chiyo, K. Matsui, Y. Murakami*, K. Yokoyama*, and E. Tamiya*

Fukumitsuya Sake Breweries
Kanazawa-shi, Ishikawa 920-8638, Japan
**Japan Advanced Institute of Science and Technology
Tatsunokuchi, Ishikawa 923-1292, Japan

We constructed the yeast-immobilized SPV device for the estimation of the rice koji. In our previous report, it took 3 hours per sample to measure samples. In this report, we improved the method for the immobilization of yeast and the structure of the flow cell. At the first, the immobilization method was changed using a microbial membrane into using an acrylamide gel which included yeast. Then, the flow cell of batch type was changed into the one of path-divided type. As the result, it became one third of the time to measure the response of a sample, and it was able to measure individual responses on the sensor chips without cross talk. We located two yeast-immobilized gel, which included Saccharomyces cerevisiae Kyokai 701 or Kyokai 9, on the sensor chip, and measured sensor responses of two types of rice koji extract with this new SPV device. As the result, two individual responses were appeared on each measurement of the two rice koji, and these four responses indicated the some difference between two rice koji.

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32.

表面光電圧法(LAPS)による集積糖類センサを用いた三成分系の同時測定 ―二酵素系セン サへの線形重回帰(MLR)法の応用―

○青木一仁、内田秀和、勝部昭明、石丸雄大、飯田武揚

埼玉大工

SIMULTANEOUS DETERMINATION FOR TERNARY MIXTURE USING INTEGRATED SACCHARIDE SENSOR BY MEANS OF LIGHT ADDRESSABLE POTENTIOMETRIC SENSOR (LAPS) -APPLICATION OF MULTIPLE LINEAR REGRESSION TO BIENZYMATIC SENSORS-

Kazuhito AOKI, Hideaki UCHIDA*, Teruaki KATSUBE**, Yoshihiro ISHIMARU, Takeaki IIDA

Department of Functional Materials Science, * Department of Electrical and Electronic Systems, ** Department of Information and Computer Sciences, Faculty of Engineering, Saitama University, 255 Shimo-okubo, Saitama-shi, Saitama-ken 338-857, Japan

One-chip integration of three saccharide biosensors was carried out by glucose sensors using thermophilic glucokinase immobilized on the light addressable potentiometric sensor (LAPS) chip. Since the simplified LAPS system was limited in number of sensing spots, a simpler method such as multiple linear regression (MLR), was applied to the mixture analysis of a low-concentrated sample. Thus, we treated glucose as a key product in the regression equation optimized for the bienzymatic biosensensing process. The multivariate calibrations of the samples were simultaneously illustrated by the estimated local glucose concentration. Finally, more than 0.7 of correlation coefficients were obtained between the true and the predicted sample concentrations although the linear approximation was not able to correct a few cases of inhibition.

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33.

新規BDPセンサの電気化学的及び分光学的検討

○沈珍、宇野英満、小野昇

愛媛大機分セ・愛媛大理

SYNTHESIS, ELECTROCHEMICAL AND SPECTROSCOPIC STUDIES ON A NEW CLASS OF BORON DIPYRROMETHENE BASED FLUOROIONPHORES

Zhen SHEN, Hidemitsu UNO, Noboru ONO

Advanced Instrumentation Center for Chenical Analysis and Department of Chemistry, Faculty of Science, Ehime University
Matsuyama 790-8577, Japan
Knut RURACK
Federal Institute for Materials Research and Testing (BAM)
Richard-Willstatter-Str. 11, D-12489 Berlin, Germany
Joerg DAUB
Institute of Organic Chemistry, University of Regensburg
D-93040 Regensburg, Germany

A new class of bifunctional fluorescent sensors were designed by employing the crown ether / or amino as cation / or proton recognition moiety and rigid bicyclo ring fused boron dipyrromethane (BDP) as signaling moiety, which can be transferred into benzo BDP dyes via a retro Diels-Alder reaction and lead to large red-shifts of both the absorption and fluorescence wavelength to the near infrared region. These molecular constitutions enable highly sensitive and selective sensory of analytes at different spectrometer.

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34.

機能単分子膜修飾電極上でのイオン選択的電極反応の解明

○谷口　功，原　和典，石本　仁，岩井　充，Srinivasan Rangarajan

熊本大工

ION SELECTIVITY FOR ELECTRODE REACTIONS ON FUNCTIONALIZED MONOLAYER MODIFIED ELECTRODE

Isao TANIGUCHI, kazunori HARA, Hitoshi ISHIMOTO, Mitsuru IWAI and Srinivasan RANGARAJAN

Department of Applied Chemistry and Biochemistry, Faculty of Engineering, Kumamoto University
2-39-1, Kurokami, Kumamoto 860-8555, Japan

Electrode reactions of various ionic species on pyridine-, pyrimidine-, benzene- and related thiolate modified Au(111) and Au(100) single crystal surfaces were carried out. Clear selectivity of the electrode reaction for a given ionic species depending on the modified surface was seen. Charge of the ionic species was not so important. In particular, on the benzenethiolate modified electrode surface, the electrode reaction of ferri-/fero- redox couple in acidic solution was clearly inhibited, but no inhibition was observed for the electrode reaction of ferri-/ferro-cyanide redox couple. On the other hand, by increasing the number of -SH group in the benzene ring (1,4-dithiol < 1,3,5 trithiol < 1,2,4,5 tetrathiol), ferri-/ferro redox couple showed an inhibition on the electrode reaction. On the bases of the properties of the modified electrode surfaces obtained by STM image, impedance analysis, contact angle and other date, the surface hyrophilicity (or hydration/dehydration of the ionic species) of the modified electrodes was concluded to play an important role on the electrode reaction of ferri-/ferro- redox couple.

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35.

エアギャップを利用した微小アンモニアガス電極の高速化、微小流路中への集積 化とその応用

○松儀泰明、鈴木博章、旭井亮一

筑波大物質工

FAST-RESPONDING AMMONIA GAS-SENSING ELECTRODE WITH AN AIR GAP FORMED IN A MICRO FLOW CHANNEL AND ITS APPLICATION

Yasuaki MATSUGI, Hiroaki SUZUKI, and Ryoichi ASAI

Institute of Materials Science, University of Tsukuba, 1-1-1 Tennodai, Tsukuba, Ibaraki 305-8573, Japan

A fast-responding miniature ammonia gas-sensing electrode was fabricated using an air gap formed in a micro flow channel. The system consists of two glass substrates. On one of them, the ammonia electrode was formed. An iridium oxide indicator electrode and a Ag/AgCl reference electrode were formed in a container formed with a thick-film photoresist SU-8. An electrolyte solution, 0.1 M KCl containing 0.1 M NH4Cl, was filled in the container. On another substrate, a flow channel was formed. When the two substrates are aligned and made in contact with each other, a silicone rubber layer intercalated between the two substrates forms an air gap. With an air gap of 1 mm thickness, the response of the electrode was less than 40 s for NH3 concentrations higher than 5 mM and 5 - 6 min for concentrations less than 100 ?M. Linear relationship was observed for ammonia concentrations higher than 20 μM. The system was used to construct a creatinine sensing system.

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36.

電気化学的ナノシリンジポンプ

○米山　玲、鈴木博章

筑波大物質工

ELECTROCHEMICAL NANO SYRINGE PUMP

Rei YONEYAMA and Hiroaki SUZUKI

Institute of Materials Science, University of Tsukuba, 1-1-1 Tennodai, Tsukuba, Ibaraki 305-8573, JAPAN

A micro system incorporating a chemical sensor and a syringe pump driven by an electrochemically generated hydrogen bubble is presented. The electrodes necessary for sensing and actuation were formed on a glass substrate by photolithography. Reservoirs for the internal electrolyte solution and a flow channel were formed on a silicon substrate. The two substrates were bonded to complete the system. Pumping was controlled by a bubble of hydrogen produced from the platinum working electrode for the actuator. Efficiency of formation and extinction of the bubble could be improved by platinizing the surface of the working electrode. Pumping rate could be controlled by adjusting the working electrode potential. Reproducible and reversible pumping could be achieved. An external sample solution containing Cu2+ was successfully introduced in the flow channel, which was clearly detected with the working electrode used for sensing.

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37.

長期安定保存を可能にする薄膜状銀／塩化銀の新構造・動作方式とμTASへの適 用

○鈴木博章、田浦　巧

筑波大物質工

NOVEL THIN-FILM Ag/AgCl STRUCTURE AND OPERATIONAL MODES TO REALIZE LONG-TERM STORAGE AND THEIR APPLICATION TO A μTAS

Hiroaki SUZUKI and Takumi TAURA

Institute of Materials Science, University of Tsukuba, 1-1-1 Tennodai, Tsukuba, Ibaraki 305-8573, Japan

A novel thin-film Ag/AgCl structure and modes of operation are proposed. The entire silver layer was passivated with a polyimide layer leaving four square pinholes in the polyimide layer to grow AgCl layers from there. In a mode of operation, no AgCl layer was grown in the structure prior to the first use and the AgCl layer was grown at a small constant current during operation. A lifetime of 300 h was achieved using an element with pinholes of 10 μm × 10 μm at 10 nA. In another mode of operation, AgCl was grown under the standby status. With AgCl layers grown at 1 ?A for 5 min, the element could maintain the equilibrium potential of Ag/AgCl for nearly 40 h in saturated KCl solution. The same experiments were conducted using the conventional Ag/AgCl structure. However, it was revealed that the novel modes of operation can never be applied to the conventional Ag/AgCl element. The novel Ag/AgCl element was used in a microfabricated liquid-junction reference electrode and was also applied to potentiometric sensors in a μTAS.

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38.

血中カテコールアミン類の検出を目的とした電気化学センサーシステム

○林　勝義、栗田僚二*、堀内　勉、丹羽　修、砂川賢二**

NTT環境研、NTT-AT*、国立循環器病センタ**

ELECTROCHEMICAL SENSOR SYSTEM FOR DETECTION OF CATECHOLAMINES IN BLOOD

Katsuyoshi HAYASHI, Ryoji KURITA*, Tsutomu HORIUCHI, Osamu NIWA, and Kenji SUNAGAWA**

NTT Lifestyle and Environmental Technology Labs.
3-1 Morinosato Wakamiya, Atsugi, Kanagawa 243-0198, Japan
*NTT Advanced Technology Corporation
3-1 Morinosato Wakamiya, Atsugi, Kanagawa 243-0124, Japan
**National Cardiovascular Center
5-7-1 Fujishirodai, Suita, Osaka 565-8565, Japan

We developed an electrochemical microfluidic sensing device combined with an interdigitated array electrode (IDA) for highly sensitive detection of catecholamines in blood. IDA electrode is highly sensitive to catecholamines because they are electrochemically reversible and can be amplified by an IDA electrode. This sensing device consists of two glass plates. One incorporates 3 carbon film electrodes, which are IDA, reference and counter electrodes and a flow channel. The width and depth of the flow channel were 1 mm and 20 μm, respectively. The IDA electrode has 125 pairs of microband electrodes. Each band is 1 mm long and 2 μm wide and the bands are separated by a 2 μm gap. The dopamine signal was enhanced by redox cycling even in the thin layer microfluidic channel. We achieved a detection limit lower than 1 nM at 5 μl/min.

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39.

Trienzyme/ポリジメチルシロキサン膜型センサによる酢酸、グリセロールの測定

○水谷文雄、矢吹聡一、飯島誠一郎

産総研

SIMULTANEOUS DETERMINATION OF ACETIC ACID AND GLYCEROL USING AMPEROMETRIC TRIENZYME ELECTRODES

Fumio MIZUTANI, Soichi YABUKI, Seiichiro IIJIMA

National Institute of Advanced Industrial Science and Technology, Central 6, Tsukuba, Ibaraki 305-8566, Japan

A trienzyme sensor for the amperometric determination of glycerol was prepared by immobilizing glycerokinase (GK), pyruvate kinase (PK) and pyruvate oxidase (PyOx) on a polydimethylsiloxane (PDMS)-coated electrode. GK catalyzes the phosphor-transfer between glycerol and ATP to produce ADP; PK, the phosphor-transfer between ADP and phosphoenolpyruvate to produce pyruvic acid; PyOx, the oxidation of pyruvic acid with oxygen. The oxygen consumption was monitored by using the PDMS-coated electrode without interference from the PyOx-reaction product, hydrogen peroxide. The concentration of glycerol (5 mM- 0.5 mM) could be measured from the decrease of the cathodic current at -0.4 V vs. Ag/AgCl. By combining acetate kinase with the PK/PyOx-based, ADP-sensing system, another trienzyme electrode was prepared and used for measuring the concentration of acetic acid. The two trienzyme electrodes were successively applied to the simultaneous determination of the two components in wines.

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40.

インクジェットプリンティングによる酵素パターンの作製とSECMイメージング

○平野　悠，小谷松大祐，西澤松彦，末永智一

東北大院工

SECM IMAGING OF PROTEIN MICROPATTERNS PREPARED BY USING A CONVENTIONAL INK-JET PRINTER

Yu HIRANO, Disuke Oyamatsu, Matsuhiko NISHIZAWA, and Tomokazu MATSUE

Department of Biomolecular Engineering, Graduate School of Engineering, Tohoku University, Sendai 980-8579, Japan

Most of recent bioanalytical systems based on immunologic and hybridization reactions in a mono- or bidimensional microarray format require technology that can produce arrays of spots containing biospecific molecules. We describe here the use of a commercial ink-jet printer as a tool to produce arrays of spots containing horseradish peroxidase on nylon membranes and glass slides. The activity of enzyme in each spot was evaluated with the scanning electrochemical microscopy (SECM).

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41.

電解系導入オキシダーゼカラム・FIAシステムによるL-アスコルビン酸の計測

飯田泰広、菊地拓也、○佐藤生男

神奈川工科大学・応用化学科

DETERMINATION OF L-ASCORBATE BY USING AN ELECTROLYTIC DEVICE・FIA SYSTEM WITH AN OXIDASE COLUMN

Yasuhiro IIDA, Takuya KIKUCHI, and Ikuo SATOH

Department of Applied Chemistry, Faculty of Engineering, Kanagawa Institute of Technology 1030 Shimo-Ogino, Atsugi-shi, Kanagawa-ken, 243-0292, Japan

An electrolytic device to extend a determination range for biosensing with use of oxidase was developed and introduced into flow-injection amperometric analysis system for L-ascorbate by using an immobilizing laccase column as a recognition element. The biosensing system was assembled with the plunger pump, the electrolytic device, the enzyme column unit, a flow-through type of oxygen electrode, and a pen recorder. The electrolytic device enabled to increase dissolved oxygen in the assay streams by electrolysis of the carrier (50 mM citrate buffer), and thereby, the additional oxygen attributable to electrolysis should be provided to the laccase column and should contribute an activation of the laccase reaction. This device consisted of two compartments; one, having two stainless tubing, was put in the flow system by connections of the stainless tubing with Teflon tubing of the flow-line, and the other having a platinum plate, was filled with electrolytes (carrier solution). These compartments were connected by a piece of ion-exchange membrane. To generate oxygen gas in the flow stream by electrolysis, a constant current was applied between the stainless tubing binding upstream through the system as a working electrode and platinum plate in the other compartment as a counter electrode. L-Ascorbate solutions (20 ul) with various concentrations were injected to the system without the electrolytic device and amounts of dissolved oxygen enzymatically consumed were amperometrically monitored. A linear relationship was obtained in a range of 0.25 ? 4.0 mM. On the other hand, a wider linear range of the L-ascorbate determination was obtained with use of the electrolytic device (0.25 - 10.0 mM). This study exemplified that use of the electrolytic device enabled to extend the dynamic range of L-ascorbate determination without any mediators and that the device might be applicable to other oxidase reaction.

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42.

ラッカーゼカラムと電解デバイスを組み合わせたビスフェノールAのバイオコンバー ジョン

○飯田泰広、菊地拓也、森井太一、佐藤生男

神奈川工科大学・応用化学科

BIOCONVERSION OF BISPHENOL A BY IMMOBILIZED LACCASE COLUMN IN COMBINATION WITH AN ELECTROLYTIC DEVICE

Yasuhiro IIDA, Takuya KIKUCHI, Taichi MORII, and Ikuo SATOH

Department of Applied Chemistry, Faculty of Engineering, Kanagawa Institute of Technology 1030 Shimo-Ogino, Atsugi-shi, Kanagawa-ken, 243-0292, Japan

Application of an electrolytic device to promote removal of BPA (bisphenol A) efficiently by using a laccase column was investigated. BPA is widely used in a variety of industrial and residential applications, and is suspected to be one of endocrine disrupting chemicals because it exhibits an estrogenic activity. Laccase, known as a polyphenol oxidase, enables to convert BPA to non-estrogenic active compound. In this study, an immobilized laccase column, requiring oxygen gas as an electron acceptor, was used in combination with an electrolytic device which could increase dissolved oxygen for degradation of BPA. The bioconversion system was assembled with the peristaltic pump, the electrolytic device, the enzyme column unit, a flow-through type of oxygen electrode, and a pen recorder. The electrolytic device enabled to increase dissolved oxygen in the assay stream by electrolysis of the carrier (50 mM citrate buffer). By additional amount of dissolved oxygen to the laccase column by using this device, laccase activity should be enhanced because dissolved oxygen is essential to the enzymatic oxidation and decides the ability of the catalysis. BPA solutions with various concentrations were injected to the system without the electrolytic device and amounts of dissolved oxygen enzymatically consumed were amperometrically monitored. A linear relationship was obtained in a range of 0.1 ? 1.0 mM. A wider linear relationship was obtained by introducing the electrolytic device. From the determination of BPA degradation by the laccase column based on RP-HPLC analysis, it was demonstrated that this bioconversion system could effectively remove BPA. Much more efficient degradation of BPA could be achieved by introducing the electrolytic device to the system.

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43.

チロシナーゼ固定化カーボンフェルトを利用するフロースルー型 ポリフェノールセンサ

○長谷部　靖、小林　崇、内山　俊一

埼玉工大工

FLOW-THROUGH POLYPHENOL SENSOR BASED ON TYROSINASE-IMMBOLIZED CARBON FELT

Yasushi HASEBE, Takashi KOBAYASHI, Shunichi UCHIYAMA

Department Applied Chemistry, Faculty of Engineering, Saitama Institute of Technology, 1690 Fusaiji, Okabe, Saitama 369-0293, Japan

Tyrosinase (Tyr) and electron transfer mediator (thionine, TN) were co-immobilized at the surface of porous carbon felt electrode. Tyr and TN co-immobilized CF (Tyr-TN-CF) was used as flow-through amperometric detector for catechol and phenolic compounds. Enzymatically produced o-quinone is reconverted to catechol at the CF surface by TN-assisted electrocatalytic reduction. Amplified peak currents based on the analyte recycling driven by enzymatic oxidation and TN-assisted electrochemical reduction is monitored at applied potential of ﾐ 50 mV (vs. Ag/AgCl). Among ten kinds of monophenol and o-diphenol compounds, higher sensitivity was obtained for catechol, p-cresol. Under the operational conditions (applied potential: -50 mV, flow rate: 1.3 ml/min, pH 7.0), the calibration curves of catechol and p-cresol by Tyr-TN-CF is linear up to 10 μM and with detection limit (S/N = 3) of 0.05μM and 0.14μM, respectively. No loss in the response could be observed after 40 injections of catechol (RSD < 2 %). The sensitivity was increased by TN-assisted electrochemical reduction as compared with those by Tyr-CF without TN in which o-quinones were directly reduced at the CF surface.

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44.

電気化学バイオセンサーによるウロカニン酸の濃度及び異性体比率の測定(2)

○岡村圭、小森喜久夫、立間徹、藤嶋昭

東大生研、東大院工

MEASUREMENT OF CONCENTRATION AND CIS/TRANS RATIO OF UROCANIC ACID BY AN ELECTROCHEMICAL BIOSENSOR (2)

Kei OKAMURA, Kikuo KOMORI, Tetsu TATSUMA, Akira FUJISHIMA

Institute of Industrial Science, University of Tokyo
Meguro-ku, Tokyo 153-8505, Japan
School of Engineering, University of Tokyo
Bunkyo-ku, Tokyo 113-8656, Japan

Urocanic acid (UA) in human skin absorbs ultraviolet light and changes from its trans isomer to cis isomer, which is harmful to skin. Thus an electrochemical biosensor is developed for the measurement of the concentration and the cis/trans ratio of UA, so that it can check skin conditions. However, compounds similar to UA (e.g., histamine) may interfere with the measurement. Then, a technique for the measurement of UA in the presence of an interfering species is developed.

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45.

ポリピロ−ル/オルガノポリシロキサン複合膜を用いたグルコ−スセンサの作製

○井上　茂、安澤幹人、今井信治*

徳島大工、東洋精密工業*

PREPARATION OF GLUCOSE SENSOR USING ORGANOPOLYSILOXANE/POLYPYRROLE COMPLEX FILM

Shigeru INOUE, Mikito YASUZAWA, Shinji IMAI

Department of Chemical Science and Technology, The University of Tokushima, Tokushima-shi, Tokushima 770-8506 *Toyo Precision Parts MFG. Co., Ltd., Yamatotakada-shi, Nara 635-0066, Japan

New glucose oxidase immobilized glucose sensors were prepared by the electropolymerization of 1-(6-D-gluconamidohexyl) pyrrole (GHP) and 6-(1-pyrrolyl)hexylphosphatidylcholine (PPC) on the platinum wire electrode precoated with the solution of pyrrole derivative (GHP and PPC) and polydimethylsiloxane. Although, the response of the electrode prepared from PPC was satisfactory obtained, no response was observed from the electrode of GHP. By the addition of Nafion into the precoating solution, the improvement of sensor sensitivity occurred and the electrode prepared from GHP also showed clear sensor response. Moreover, the introduction of Nafion was effective to improve the long-term stability of the enzyme immobilized electrodes. The electrode prepared from both Nafion and GHP performed excellent long-term stability. Relatively constant response current was obtained over 30 days in pH 7.4 phosphate buffer solution under the condition of 40 C measurement and storage temperatures.

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46.

銅ナノ微粒子分散炭素薄膜の作製と糖類検出への応用

由 天艶、丹羽 修、富田 雅人、安藤 洋*、廣野 滋**

NTT生活環境研究所, *NTT-AT, **NTT-Afty

PREPARATION OF NOVEL HIGHLY DISPERSED COPPER NANOPARTICLES IN GRAPHITE-LIKE CARBON FILM AND THE APPLICATION FOR GLUCOSE DETECTION

Tianyan YOU, Osamu NIWA, Masato TOMITA, Hiroshi ANDO*, Shigeru HIRONO**

NTT Lifestyle and Environmental Technology Labs, 3-1 Morinosato, Wakamiya, Atsugi, Kanagawa 243-0198, Japan *NTT Advanced Technology Corporation, 3-1 Morinosato, Wakamiya, Atsugi, Kanagawa 243-0198, Japan **NTT AFTY Corporation, 4-16-30 Shimorenjyaku, Mitaka, Tokyo 181-0013, Japan

We used a radio frequency (RF) sputtering method for forming a novel copper nanoscale particles highly dispersed in graphite-like carbon film (Cu-NRC) by co-sputtering copper and carbon. The preparation is very simple, controllable and reproducible. The film structure was investigated by XPS and TEM measurements. There is 4.5% copper atom concentration in the film and the size of copper nanoparticles is about 4 ~ 5 nm. The copper in the Cu-NDC film is of oxide states. The Cu-NDC film electrodes are highly electrocatalytic with regard to the electrooxidatoin of glucose with good stability.

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47.

高分子交互累積膜法による過酸化水素検出型尿酸センサの開発

○斉木秀和、星　友典、安斉順一

東北大院薬

AMPEROMETRIC SENSORS BASED ON POLYELECTROLYTE MULTILAYER FILMS FOR URIC ACID

Hidekazu SAIKI, Tomonori HOSHI, Jun-ichi ANZAI

Graduate School of Pharmaceutical Sciences, Tohoku University, Aoba-ku, Sendai 980-8578, JAPAN

Platinum electrodes coated with a poly(allylamine)/poly(vinylsulfate) film can be used for detecting H2O2 selectively in the presence of the possible interfering agents such as ascorbic acid, uric acid. Uricase (UOx) was then deposited on the polyelectrolyte multilayer films with poly(allylamine) through electrostatic interaction. The response current for uric acid increased with increasing the number of layers of UOx. In the presence of ascorbic acid, we detected uric acid over the concentration range of 10-6 -10-3 M successfully. The stability of the sensor was checked by measuring uric acid for 30 days. The response of the sensor to uric acid was decreased by 40 % from the original activity.

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48.

血清中のＮＯ迅速アッセイ電気泳動チップの予備的検討

○脇田慎一、宮道 隆、永井秀典、黒澤 茂、吉田康一、二木鋭雄

産総研

PRELIMINARY STUDY ON HIGH THROUGHPUT NO ASSAY IN BLOOD SERUM USING MICROCHIP BASED CAPILLARY ELECTROPHORESIS

Shin-ichi WAKIDA, Takashi MIYADOU, Hidenori NAGAI, Shigeru KUROSAWA, Yasukazu YOSHIDA and Etsuo NIKI

Human Stress Signal Research Center, National Institute of Advanced Industrial Science and Technology (AIST), Ikeda, Osaka 563-8577 , Japan

We successfully demonstrated conventional capillary electrophoresis (CE) assay for NO metabolites in deproteinized serum within 9 min with a novel buffer solution to control micro- fluidics of reverse electroosmotic flow (EOF) and stacking pre-concentration. As we also preliminarily studied high throughput CE assay for the NO metabolites using microchip based CE technology, we achieved only 14 second assay in 50-fold concentrated standard solution to make some control of microfluids.

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49.

ナノ白金微粒子分散炭素薄膜電極のバイオセンサとして特性

○丹羽　修、Tianyan You、富田　雅人、岩崎　弦、堀内　勉、廣野　滋

NTT生活環境研究所、NTTアフティ

ELECTROCHEMICAL PROPERTIES OF NANO-Pt CLUSTER DISPERSED CARBON FILM ELECTRODES AND THEIR APPLICATION FOR BIOSENSORS

Osamu NIWA, Tianyan YOU, Masato TOMITA, Yuzuru IWASAKI, Tsutomu HORIUCHI, Shigeru HIRONO

NTT Lifestyle & Environmental Technology Laboratories
3-1 Morinosato, Wakamiya, Atsugi, Kanagawa 243-0198 Japan
NTT Afty Corporation
4-16-30, Shimorenjyaku, Mitaka, Tokyo 181-0013 Japan

Nanoscale platinum metal cluster array electrodes in the conductive carbon filmwas prepared by a simple RF sputtering method. The content of Pt and controlable and each cluster is about 2-3 nm in diameter. The Pt-cluster dispersed carbon film has high electrocatalitic activity and good stability to H+ reduction, dioxygen reduction and hydrogen peroxide oxidation. We optimized Pt-cluster content to obtain highest electrocatalitic activity and applied as a detector for biosensor by modifying the film with enzymes such as glucose oxidase.

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特別講演

人工選択系による新機能抗体の創製

○熊谷 泉

東北大学大学院工学研究科

GENERATION OF NOVEL ANTIBODIES USING ARTIFICIAL SELECTION SYSTEM

Izumi KUMAGAI

Department of Biomolecular Engineering, Graduate School of Engineering, Tohoku University, Aoba-ku, Sendai 980-8579, Japan

Antibody molecules, also called immunoglobulins, are proteins that play a significant role in immune system, and one of the major immunoglobulins in vivo, IgG, can recognize their targets with high specificity and affinity, which utilize for various fields, e.g. diagnostics, biosensors, cellular and molecular biology, and immunotherapy. Antibodies can be regarded as a protein engineering system perfected by nature for the generation of a virtually unlimited repertoire of complementary molecular surfaces, which was often called complementarity determining region (CDR) and created by two variable domains (VH and VL), suggesting that construction of artificial gene libraries and improvement of selection system in vitro makes it possible to create novel artifical antibodies. Here I would report selection and preparation of artificial antibody molecules using bacterial system and also their application to biomaterials will be introduced.

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50.

ダイヤモンド水素終端表面におけるハロゲンイオンの影響

○堺俊克、荒木裕太、金澤啓史、宋光燮、梅沢仁、立木実、川原田洋

早大理工、CREST科技団

EFFECT OF HAROGEN ION TO HYDROGEN-TERMINATED DIAMOND SURFACE

Toshikatsu SAKAI, Yuta ARAKI, Hirofumi KANAZAWA, Kwan-Soup SONG, Hitoshi UMEZAWA, Minoru TACHIKI and Hiroshi KAWARADA

*Department of Functional Materials Science
**Department of Information and Computer Sciences ,Faculty of Engineering, Saitama University
255 Shimo-okubo, Urawa-shi, Saitama-ken 338-8570, Japan

Using the advantages of diamond, such as chemical stability, wide potential window, and biocompatibility, diamond surface channel FETs operated in electrolyte solutions is fabricated. In this FET, diamond surface is in contact with the electrolyte solution. From the results in various solutions, it is observed that the FET was insensitive to pH values, but sensitive to the concentration of halogen ions. In KCl, NaCl, KBr solutions, the sensitivity of the FET is approximately 30 mV/decade.　In KI solutions, the response of the FET is greater than Cl- or Br- ion. These results indicate that hydrogen-terminated diamond surface has the sensitivity to the halogen ions, and the effect of iodide ion is stronger than the other measured solutions.

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51.

チロシナーゼ修飾ダイヤモンド電極によるビスフェノールAのセンシング

○野津英男、立間　徹*、藤嶋　昭

東大院工、東大生研*

SENSING OF BISPHENOL-A BY USING A TYROSINASE-MODIFIED DIAMOND ELECTRODE

Hideo NOTSU, Tetsu TATSUMA*, Akira FUJISHIMA

Department of Applied Chemistry, School of Engineering, University of Tokyo
7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
*Institute of Industrial Science, University of Tokyo
4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan

Highly boron doped conductive diamond is well known as an electrode material suitable for the quantitative detection of a small amount of chemical compounds. However, as the diamond electrode has low catalytic activities, detectable compounds are somewhat limited. Therefore, we modified the diamond electrode with enzyme. By using this enzyme-modified diamond electrode, we tried to detect enzyme substrates, which could not be detected by the bare diamond electrode. On the other hand, most of phenol derivatives are known as harmful compounds. In particular, some of them (e.g., bisphenol-A) are regarded as endocrine disruptors that might cause abnormal feminizing responses of animals. Thus, detection and determination of phenol derivatives are very important. For this purpose, a tyrosinase-modified diamond electrode was developed in the present work.

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52.

ダイヤモンドマイクロ電極の電気化学分析

○Olivia Herlambang, Bulusu V. Sarada, Tata N. Rao, 藤嶋 昭

東大工

ELECTROANALYTICAL APPLICATIONS OF HIGHLY BORON-DOPED DIAMOND MICROFIBER ELECTRODE

Olivia HERLAMBANG, Bulusu V. SARADA, Tata N. RAO, Akira FUJISHIMA

Department of Applied Chemistry, Undergraduate School of Engineering, The University of Tokyo Hongo, Bunkyo-ku, Tokyo 113-8656, Japan

Highly boron-doped diamond (BDD) microfiber electrodes were fabricated and characterized by the use of Scanning Electron Microscopy (SEM), Raman spectroscopy, and cyclic voltammetry. These microfiber electrodes were examined for several applications as biosensors in electroanalysis. Dopamine, a neurotransmitter, was detected at overoxidized poly pyrrole (OPPy)-modified BDD microfiber electrodes. OPPy film attracts dopamine cations and rejects ascorbate anions, allowing the detection of dopamine with high selectivity and stability in the presence of large excess of ascorbic acid. The limit of detection (LOD) of dopamine was 0.5 nM (S/N = 3) and the calibration curves were linear in the range from 1 nM to 100 nM. The LOD was one order lower than that observed for carbon microfiber electrodes. Glucose was determined by detecting enzymatically produced H2O2 at Ir-GOx-BDD microfiber electrodes, at ?0.3 V vs SCE. The calibration curve plotted from the amperometric measurements was linear in the range of 1-15 mM.

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53.

イリジウム担持ダイヤモンド複合電極を用いたグルコースセンサー

○佐々木典子、Bulusu V. Sarada、寺島千晶、Tata N. Rao、藤嶋　昭

東大院工

ENZYMATIC DETECTION OF GLUCOSE AT IRIDIUM-MODIFIED DIAMOND ELECTRODES USING FLOW INJECTION ANALYSIS

Noriko SASAKI, Bulusu V. SARADA, Chiaki TERASHIMA, Tata N. RAO, Akira FUJISHIMA

Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan

Detection of glucose at iridium-modified diamond (Ir-BDD) electrode by use of a glucose oxidase immobilized enzyme reactor with flow injection analysis is demonstrated. Enzymatically produced H2O2 was detected at ?0.14 V vs. Ag/AgCl with no interference from other electroactive compounds at Ir-BDD due to the high catalytic activity of iridium for the reduction of H2O2. The limit of detection (LOD) for glucose was 10 microM and the calibration curve was linear in the range of 10 microM to 5 mM (R2 = 0.999). The results demonstrate the stability of electrode during the experiment with an RSD of 5 % for 50 injections of 1 mM glucose.

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54.

Electrochemical detection of nitrate at Cu-modified diamond electrodes

Tata N. RAO, Bulusu V. SARADA and Akira FUJISHIMA

Department of Applied Chemistry, School of Engineering The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan

Copper-modified boron-doped diamond electrodes were examined for the electrochemical detection of nitrate by reducing it in acidic solution. The detection of nitrate was performed by cyclic voltammetry and flow-injection analysis. Diamond being a unique material for the electrochemical deposition of Cu clusters, it acts as an excellent support for the detection of nitrate with high sensitivity. Diamond also allows complete stripping and re-deposition of Cu metal clusters, which enables the rapid renewal of fresh Cu surface for reproducible detection of nitrate.

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55.

ELECTROCHEMICAL DETECTION OF UNDERIVATIZED AMINO ACIDS BY HPLC USING COPPER MODIFIED-DIAMOND ELECTRODE

Tribidasari A. IVANDINI, Bulusu V. SARADA, Tata N. RAO and Akira FUJISHIMA

Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo 113-8656, Japan

Copper modified-diamond electrode was examined for electrochemical detection of amino acids (histidine, alanine and arginine) under flow conditions. At detection potential of 0.55 mV vs. Ag/AgCl/1 M LiCl and NaOH as mobile phase (pH 13), the amino acids were good sensitivity detected with the limit of detection (S/N=3) between 2 nM to 100 nM and high stability with an RSD value under 3 %. The conditions were optimized for the simultaneous amperometric detection of amino acids detection after HPLC separation.

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56.

抗体アレイチップの高感度電気化学イメージング法の開発

○本地直美*，平野悠**，我孫子裕子**，小谷松大祐**， 西澤松彦**，末永智一**，牛澤幸司***，川端荘平****

東北大院生命*，東北大院工**，第一化学薬品（株）***，（株）アイ・ティ・リ サーチ****

DEVELOPMENT OF HIGH SENSITIVITY ELECTROCHEMICAL IMAGING SYSTEM AND APPLICATION TO MALTI-IMMUNOASSAY

Naomi MOTOCHI*, Yu HIRANO**, Yuko ABIKO**, Daisuke OYAMATSU**, Matsuhiko NISHIZAWA**, Tomokazu MATSUE**, Kouji USHIZAWA***, Souhei KAWABATA****

*Department of Molecular Immunology, Graduate School of Life Science, Tohoku University, Sendai 980-8577 **Department of Biomolecular Engineering, Graduate School of Engineering, Tohoku University, Sendai 980-8579 ***Daiichi Pure Chemicals co., Ltd. Chuo-ku, Tokyo 103 ****I. T. Research Co., Ltd. Sendai 981-3203 , Japan

In this study, we have developed an immunoassay system based on the scanning electrochemical microscopy (SECM) for detection of C-reactive protein (CRP) in the pg/mL level. For this purpose, we fabricated an antibody array chip by spotting antibodies on a glass substrate. After forming a sandwich structure with an enzyme-labeled second antibody, the electrochemical immunoassay was conducted by imaging the enzymatically amplified current signal at the antibody spots on the chip.

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57.

心筋細胞の局所パターニングによる新規バイオアッセイ系の構築

○梶　弘和、高橋　淳、小谷松大祐、西澤松彦、末永智一


東北大院工

DEVELOPMENT OF NOVEL BIOASSAY SYSTEM USING MICROPATTERNED CARDIAC MYOCYTES

Hirokazu KAJI, Atsushi TAKAHASHI, Daisuke OYAMATSU, Matsuhiko NISHIZAWA, Tomokazu MATSUE

Department of Biomolecular Engineering, Graduate School of Engineering, Tohoku University, Sendai 980-8579, Japan

The patterning of cardiac myocytes on a micron scale was achieved by microcontact printing of fibronectin onto a hydrophobically pretreated glass substrate. The patterned cardiac myocytes conjugated with each other by forming a gap junction, as judged from the synchronized Ca2+ transition over the pattern, and thus simultaneously contracted. The dynamic change of Ca2+ concentration within the patterned tissue was quantitatively analyzed during the successive contraction and relaxation using a Nipkow-type high-speed confocal microscope. Futhermore, the patterning of cardiac myocytes on an indium tin oxide (ITO) microelectrodes array was also attempted for developing novel bioassay devices.

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58.

オンチップ型アレルギー診断システムの開発

○林　泰圭、太田裕子、竹山春子、松永　是

東京農工大工

DEVELOPMENT OF A ON-CHIP TYPE ELECTROCHEMICAL DETECTION SYSTEM FOR HISTAMINE

Tae-Kyu LIM, Hiroko OHTA, Haruko TAKEYAMA, Tadashi MATSUNAGA

Department of Biotechnology, Tokyo University of Agriculture and Technology, Koganei, Tokyo 184-8588, Japan

Ferrocenecarboxylic acid (Fc) conjugated with immunoglobulin G (IgG) antibody (Fc-IgG) was prepared and used as a novel analytical reagent for histamine detection. The system consists of the cation exchange resin coated matrix column on PMMA (poly methylmethacrylate) plate and the flow cell for electrochemical detection of Fc-IgG. The assay yielded a linear relationship between signal and histamine concentration in the range of 0 - 200 microgram/ml. This simple technique permits the assay of histamine within 2 min. This electrochemical flow immunoassay requires only minute quantities of serum and generates highly reproducible results.

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59.

抗原抗体反応を用いたリアクター・ディテクター分離型センサの開発（II）

○濱田浩幸、大賀敬介、安澤幹人

徳島大工

DEVELOPMENT OF REACTOR/DETECTOR DEVIDED ANTIBODY SENSOR (II)

Hiroyuki HAMADA, Keisuke OGA, Mikito YASUZAWA

Department of Chemical Science and Technology, The University of Tokushima, Tokushima-shi, Tokushima 770-8506 , Japan

Reactor/detector devided antibody sensing system was developed using two monoclonal IgG class anti-rat transferrin antibodies (15C2H3 and 22A06D2). Agarose resin containing hydrazide was applied to immobilize 22A06D2 and ferrocene polymer was labeled to 15C2H3. After the sandwich formation (agarose resin=antibody-antigen-antibody=ferrocene polymer) was constructed proportionally to the transferrin concentration, the reactor was treated with acidic solution and the antibody=ferrocene polymer was released from the the reactor in order to be measured amperometrically at the detector. The relationship between the transferrin concentration and sensor response was measured in the range of 0 to 300 ng cm-3 and relatively good calibration curve was obtained. The antibody immobilized agarose resin was able to reuse at least 5 times.

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60.

生体物質検出用酵素固定化マイクロおよびナノ電極を含むマイクロ流体構造の作製

○安川智之，Andrew GLIDLE，野村昌行，Jonathan M. COOPER

グラスゴー大工，旭化成(株）

MICROMACHINED STRUCTURES INCLUDING FUNCTIONALISED MICRO AND NANO ELECTRODES FOR IMMOBILISING ENZYMES USED IN THE DETECTION OF METABOLITES

Tomoyuki YASUKAWA, Andrew GLIDLE, Masayuki NOMURA, Jonathan M. COOPER

Bioelectronics Research Centre, Department of Electronics & Electrical Engineering, Oakfield Ave, University of Glasgow, Glasgow G12 8QQ U.K.
Central Technology Laboratory, ASAHI KASEI CORPORATION
2-1, Samejima, Fuji, Shizuoka 416-8501, Japan

We have fabricated a micromachined structure comprising a picolitre scale (ca. 600 pL) analytical chamber to electrochemically measure cellular metabolites by enzyme assays. The structure was fabricated using a negative photoresist, SU-8, and silicone sealant. The chamber portion of the device contained three gold microelectrodes and six nanoelectrodes. Microfluidic features of the device included a number of inlet/outlet channels to introduce a single cell, enzymes and reagents into the chamber. The electrochemical response was characterized by generator-collector voltammetry. b-nicotinamide adenine dinucleotide, reduced form (NADH) which is required as a cofactor in a large number of dehydrogenese based biosensors was detected using on one of microelectrode in chamber is also discussed for utilising the device as an enzyme based biosensor.

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61.

コラーゲンを用いた微生物チップの作製と電気化学計測

○彼谷高敏，長峯邦明，小谷松大祐，西澤松彦，末永智一

東北大院工

FABRICATION OF A MICROBIAL CHIP USING COLLAGEN FOR ELECTROCHEMICAL BIOASSAY

Takatoshi KAYA, Kuniaki NAGAMINE, Daisuke OYAMATSU, Matsuhiko NISHIZAWA, Tomokazu MATSUE

Department of Biomolecular Engineering, Graduate School of Engineering, Tohoku University, AramakiAoba07, Aoba-ku, Sendai 980-8579, Japan

Microbial chips with immobilized living bacteria have been studied as new sensing devises for bioactive chemicals. These chips are based on detection of activity changes of immobilized bacteria upon exposure to hazardous materials. In the present study, we fabricated microbial chips with an E.coli / collagen microspot. The chips was immersed into a buffer solution containing Fe(CN)64- and the respiration activity of the E.coli spot was investigated using scanning electrochemical microscopy (SECM). The SECM images based on oxidation of Fe(CN)64- changed drastically by adding 20mM D-glucose to the solution. The effects of antibiotics such as streptomycin was also studied.

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62.

マイクロチャンネルチップを用いた誘電泳動による単一細胞操作

○尾形　幸子，高橋　透，安川　智之、小谷松　大祐，西澤　松彦，末永　智一

東北大院工・東北大学際セ・グラスゴー大

Dielectrophoretic Manipulation of Single Cells in a Micro-channel Chip

S. Ogata(a), T. Takahashi(b), T. Yasukawa(c), D. Oyamatsu(a), M. Nishizawa(a), T. Matsue(a)
(a) Department of Biomolecular Engineering, Graduate School of Engineering, Tohoku University, 07Aramaki-Aoba, Aoba-Ku, Sendai 980-8579, Japan (b) Center for Interdisciplinary Research, Tohoku University, 07Aramaki-Aoba, Aoba-Ku, Sendai, 980-8578, Japan　 (c) Bioelectronics　Research Centre, Department of Electronics & Electrical Engineering, University of Glasgow, Glasgow G12 8QQ, UK

Handling the single cell, which is the minimum unit of the life, is important for diagnostics and biotechnology. Inhomogeneous, high-frequency ac electric fields can be used to manipulate molecules and particles by dielectrophoresis. Integration and miniaturization of various bioanalytical systems on a microchip has been a recent trend in biotechnology. Miniaturization allows such field minima to be created on a scale suitable for handling single, small objects, such as single cells. In the present study, by using the semiconductor processing technique, We integrate dielectrophoretic modular elements and microchannels to manipulate particle and cell. We utilized the combination of siloxane polymer with glass plates for the chip preparation. Siloxane polymer membrane is a transparent, hydrophobic elastomer in which micro channels can be formed by curing the polymer with a master that contains the desired microchip features. A cell suspension solution was injected to the device, and transported through the flowchannel by using a syringe pump. We placed an interdigitated electrodes array within the channel, which would work as an unit for capturing a cell by the electrophoretic force. If dielectric properties of individual cells are sufficiently different, the cell can be separated. We are now attempting the separation of E. coli and yeast. We show how this device can be used as the basic tool in a particle sorter. The on-line electrochemical analysis of the intracellular materials in the single cell level is our final objective.

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