WO2002013296A1 - Oxyde composite pour electrode oxydoreductrice et materiau de collecteur de pile a combustible a electrolyte solide, procede de preparation de ceux-ci et pile a combustible a electrolyte solide - Google Patents

Oxyde composite pour electrode oxydoreductrice et materiau de collecteur de pile a combustible a electrolyte solide, procede de preparation de ceux-ci et pile a combustible a electrolyte solide Download PDF

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Publication number
WO2002013296A1
WO2002013296A1 PCT/JP2001/006488 JP0106488W WO0213296A1 WO 2002013296 A1 WO2002013296 A1 WO 2002013296A1 JP 0106488 W JP0106488 W JP 0106488W WO 0213296 A1 WO0213296 A1 WO 0213296A1
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WO
WIPO (PCT)
Prior art keywords
fuel cell
air electrode
composite oxide
solid electrolyte
electrolyte fuel
Prior art date
Application number
PCT/JP2001/006488
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English (en)
Japanese (ja)
Inventor
Eisaku Suda
Original Assignee
Anan Kasei Co., Ltd.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Anan Kasei Co., Ltd. filed Critical Anan Kasei Co., Ltd.
Priority to AU2001276693A priority Critical patent/AU2001276693A1/en
Publication of WO2002013296A1 publication Critical patent/WO2002013296A1/fr

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • H01M4/9025—Oxides specially used in fuel cell operating at high temperature, e.g. SOFC
    • H01M4/9033—Complex oxides, optionally doped, of the type M1MeO3, M1 being an alkaline earth metal or a rare earth, Me being a metal, e.g. perovskites
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/016—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on manganites
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/50—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on rare-earth compounds
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8605—Porous electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
    • H01M4/8882—Heat treatment, e.g. drying, baking
    • H01M4/8885—Sintering or firing
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0215—Glass; Ceramic materials
    • H01M8/0217—Complex oxides, optionally doped, of the type AMO3, A being an alkaline earth metal or rare earth metal and M being a metal, e.g. perovskites
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1007—Fuel cells with solid electrolytes with both reactants being gaseous or vaporised
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a composite oxide for an air electrode and a raw material for a current collector of a solid oxide fuel cell, a method for producing the same, and a solid oxide fuel cell.
  • the solid oxide fuel cell has a high operating temperature of 100 ° C and high waste heat obtained from the battery, high power generation efficiency can be obtained by using the waste heat for the steam turbine. In addition, cold and warm heat can be supplied by using an absorption refrigerator. Therefore, solid electrolyte fuel cells are expected to be used in a wide range of applications, from small power sources for cogeneration to large power sources for thermal power.
  • Lanthanum manganite doped with Sr and Ca is used for the air electrode and current collector of the solid oxide fuel cell.
  • the lantern manganite has various compositions. For example, La 0 with a part of the A site lanthanum replacement with 10 mole 0/0 of Sr of lanthanum manganite Naito (LaMn0 3 + 5). 9 Sr 0. Substituted with MNOG + s or 20 mole 0/0 Ca La 0. 8 Ca 0 was. 2 ⁇ 3 + ⁇ is yttria stabilized Jirukoyua (hereinafter, abbreviated as YSZ) because it has a thermal expansion coefficient close to the thermal expansion coefficient of the solid oxide fuel cell air Goku ⁇ Used for current collectors.
  • YSZ yttria stabilized Jirukoyua
  • the heat cycle shrinkage phenomenon is caused by the densification of the lanthanum manganite. This may be because the lanthanum manganate undergoes a phase change due to the release and absorption of oxygen due to the movement of the A-site and B-site metal elements, thereby increasing the diffusion rate and promoting sintering.
  • the shrinkage phenomenon causes a stress in the cell body, which causes cracks in the air electrode and the current collector and causes separation from the electrolyte. If the air electrode and the current collector are cracked or separated, the performance of the electrode and the current collector is reduced, the power generation capacity is reduced, and the operation of the solid oxide fuel cell is stopped. In addition, since the air electrode and the current collector are in close contact with the solid electrolyte substrate, different thermal expansion coefficients cause the same cracking and peeling as described above. Disclosure of the invention
  • An object of the present invention is to suppress a contraction phenomenon caused by a thermal cycle of a solid oxide fuel cell, and have a thermal expansion coefficient substantially equal to that of YSZ, which is an electrolyte of the solid oxide fuel cell, so that cracking and peeling can be suppressed.
  • Another object of the present invention is to provide a composite oxide for a cathode and a raw material for a current collector of a solid oxide fuel cell having high sinterability and improved conductivity, and a method for producing the same.
  • Another object of the present invention is to provide a long-life solid oxide fuel cell in which shrinkage of the air electrode and the current collector during thermal cycling is suppressed and prevented, and cracking and peeling are suppressed.
  • L ai —X — y A x L n y Mn z 03 + 5 (where A represents Ca and / or Sr, and Ln is selected from the group consisting of Sm, Gd and Y.
  • X, y and z are 0.3 ⁇ x ⁇ 0.6, 0 ⁇ y ⁇ 0.3 s and 1.5 ⁇ z ⁇ 4.5).
  • a composite oxide for a cathode of a fuel cell and a raw material for a current collector is provided.
  • a method for producing the above-mentioned composite oxide, which is characterized by mixing and sintering, is provided.
  • a solid oxide fuel cell using the above-described composite oxide for an air electrode, a Z, or a current collector.
  • Composite oxides of the present invention is intended to be used as a raw material of the raw material ⁇ Pi collector of the air electrode used in the solid electrolyte type fuel cell, La i _ x _ y A x Ln y ⁇ ⁇ ⁇ 3 + ⁇ Is a lanthanum-manganese-based composite oxide represented by the following composition formula (hereinafter may be referred to as “the oxidized product of the present invention”).
  • ⁇ in the above formula represents Ca and Bu or Sr
  • Ln represents at least one selected from the group consisting of Sm, Gd and Y force
  • x, y and ⁇ 0.3 ⁇ x ⁇ 0.6, 0 ⁇ y ⁇ 0.3, 1.5 ⁇ z ⁇ 4.5
  • no sintering due to thermal cycling occurs up to the operating temperature of the solid oxide fuel cell up to 1000 ° C
  • shrinkage due to thermal cycling The phenomenon can be suppressed.
  • the thermal expansion coefficient of the oxidized product of the present invention is a solid oxide fuel cell.
  • the thermal expansion coefficient of YSZ used for the electrolyte of the present invention is almost the same.
  • the addition of Sr, Z, or Ca as the element A aims at suppressing thermal cycle shrinkage.
  • the value of X is preferably 0.3 ⁇ x ⁇ 0.6, particularly preferably 0.4 ⁇ X ⁇ 0.5 in the case of LaSr system. In the LaCa system, it is preferably 0.4 ⁇ x ⁇ 0.6, particularly preferably 0.4 ⁇ x ⁇ 0.5.
  • a part of La can be replaced with Sm, Gd or Y for the purpose of adjusting the coefficient of thermal expansion. Even without replacement, if the values of X and z are in appropriate ranges, the coefficient of thermal expansion can be made substantially equal to the coefficient of thermal expansion of YSZ. If it is necessary to adjust the thermal expansion coefficient in a more strict sense, La can be partially replaced with rare earth.
  • the ionic radius of rare earth elements decreases with increasing atomic number due to the lanthanide contraction phenomenon. Among the rare earth elements, La 3 + has the largest ionic radius.
  • the substitution amount is 0 and y ⁇ 0.3, even if La is partially replaced with Sm, Gd, or Y, the dioptric force structure can be maintained. This facilitates a stable thermal expansion behavior without affecting the electronic structure of ⁇ . However, at y> 0.3, the veropskite structure cannot be maintained, and stable thermal expansion behavior is not exhibited.
  • the value of z indicating the amount of Mn is 1.5 ⁇ z ⁇ 4.5, preferably 2.0 ⁇ z ⁇ 4.0, and more preferably 2.5 ⁇ z ⁇ 3.5. If the value of z is less than 1.5, the coefficient of thermal expansion becomes too large compared to that of YSZ, and if it exceeds 4.5, the coefficient of thermal expansion becomes too small, which is not preferable.
  • composition of the oxide of the present invention is not particularly limited as it satisfies the above composition formula for example La 0. 6 Ca 0. 4 Mn was 5 O 3 + There La 0. 6 Ca 0. 4 Mn 2. 4 ⁇ 3 + ⁇ ⁇ La 0. 6 Ca 0. 4 Mn 3. i 0 3 + There La 0. 6 Ca 0. 4 Mn 4. 2 O 3 + There La 0. 6 Sr 0. 4 Mn ⁇ 5 O 3 + La 0. 6 Sr 0. 4 Mn 2. 5 0 3 + There La 0. 6 Sr 0. 4 Mn 3. 3 0 3 + There La 0. 6 Sr 0. 4 Mn 4. 4 0 3 + ⁇ etc. No.
  • the porosity of the oxide of the present invention is such that an oxide having a porosity of about 30% or less can be produced, and preferably 10% or less.
  • the oxide of the present invention for the air electrode and the current collector of a solid electrolyte battery, there are known methods, for example, a production method by CVD or EVD, a method of applying an oxide paste and then firing. Used.
  • ⁇ 1 La -x- y A x Ln y Mn z 0 3 + s
  • the raw material of the complex oxidized product in which z is 1 used in the production method of the present invention can be produced by a known method such as a powder mixing method, a coprecipitation method, and a sol-gel method.
  • MnO manganese oxide to be mixed with the composite oxide raw material
  • MnO manganese oxide
  • Mn 2 O 3, Mn 3 O 4, Mn0 2 , and the like all these Mn 3 0 4 becomes by heating to 940 ° C or higher in air
  • this structure is for Mn 3 0 4 is preferably used in a stable even at room temperature! / ⁇ .
  • a method using a commercially available mixer, or a method of experimentally using a mortar or the like can be adopted. .
  • the conditions can be appropriately selected. At this time, if the mixing is not uniform, the thermal expansion coefficients of the sintered portions will be different, causing cracks in the sintered body, and the difference in thermal expansion coefficient from YSZ will increase.
  • the temperature for sintering the mixture of the composite oxide raw material and manganese oxide is usually 1000 to 1500 ° C, preferably 1200 to 1500 ° C, and more preferably 1300 to 1500.
  • C. Sintering temperature is 1000. If it is less than C, it takes a long time to obtain a composite oxide having a low porosity. In particular, if using a non Mn 3 0 4 as manganese oxide is undesirable because there is a possibility that there is a manganese oxide not fit will Mn 3 O 4 at temperatures below 1000 ° C.
  • the sintering time can be appropriately selected depending on the sintering temperature. Usually, when the sintering time is 2 hours or more, a sintered body having a porosity of 30% or less is obtained. In order to obtain a sintered body having a porosity of 10% or less, it is preferable to set a sintering time of 4 hours or more. '
  • the oxide of the present invention may be used for the air electrode and / or the current collector, and the preparation of the air electrode and the current collector can be performed by a known method. . Since the oxide of the present invention has the specific composition described above, it suppresses the contraction phenomenon caused by the thermal cycle of the solid oxide fuel cell, and has a thermal expansion coefficient substantially equal to that of YSZ, which is the electrolyte of the solid oxide fuel cell. Equally, cracking and peeling can be suppressed. Further, the oxide of the present invention has high sinterability and improved conductivity, and thus is useful as a raw material for an air electrode and a current collector of a solid oxide fuel cell. , Since the solid oxide fuel cell of the present invention uses the oxide of the present invention for an air electrode and / or a current collector, a long life is maintained based on the characteristics of the oxide.
  • the obtained sintered body was cut into a size of 5 mm in length, 5 mm in width and 20 mm in length using a diamond cutter, and measured using a differential type thermal expansion meter (TD-5000S) manufactured by Mac Science. .
  • the thermal expansion coefficient of the prepared powder was measured.
  • the density of the sintered body cut into the same size was measured by a caliper method, and the porosity was obtained by the following equation. Table 1 shows the results.
  • Porosity (%) (1—measured density (gZcm 3 ) / theoretical density (gZcm 3 )) ⁇ 100
  • a sintered body was obtained in the same manner as in Example 8 except that Mn 3 O 4 was not mixed, and each measurement was performed. Table 1 shows the results.
  • the operating conditions were as follows: 600 to: L100 ° C in the range of 5 ° C / Z for the temperature rise / fall rate, during which the temperature was maintained at 1000 ° C for 1 hour during the temperature rise. After 10 heat cycles, the air electrode surface was observed by SEM.
  • the evaluation of the test was performed by obtaining the maximum power density at 1000 ° C.
  • the relationship between voltage and current was measured using a voltmeter (Advantest, R8240) and a voltage / current generator (Adpantest, R6142), and the maximum output density was determined by considering the electrode area. .
  • the results are shown in Tables 2 and 3.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Ceramic Engineering (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Structural Engineering (AREA)
  • Organic Chemistry (AREA)
  • Thermal Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Inert Electrodes (AREA)
  • Fuel Cell (AREA)
  • Compositions Of Oxide Ceramics (AREA)

Abstract

La présente invention concerne un oxyde composite destiné à une électrode oxydoréductrice et un matériau de collecteur de pile à combustible à électrolyte solide, qui comprend un oxyde composite représenté par La1-x-yAxLnyMnzO3+δ. Dans cette formule A représente Ca et/ou Sr, Ln représente au moins un des éléments sélectionnés parmi Sm, Gd et Y, 0,3 ≤ x ≤ 0,6, 0 ≤ y ≤ 0,3 et 1,5 ≤ z ≤ 4,5. Cet oxyde composite est supprimé par le phénomène de rétraction causé par les cycles thermiques d'une pile à combustible à électrolyte solide, est réduit dans la fragmentation ou l'exfoliation de celui-ci, présente des propriétés de frittage améliorées et possède une conductivité améliorée.
PCT/JP2001/006488 2000-08-04 2001-07-27 Oxyde composite pour electrode oxydoreductrice et materiau de collecteur de pile a combustible a electrolyte solide, procede de preparation de ceux-ci et pile a combustible a electrolyte solide WO2002013296A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU2001276693A AU2001276693A1 (en) 2000-08-04 2001-07-27 Composite oxide for air electrode and material of collector of solid electrolytefuel cell, method for preparation thereof, and solid electrolyte fuel cell

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2000236809A JP2002053374A (ja) 2000-08-04 2000-08-04 固体電解質型燃料電池の空気極用及び集電体原料用複合酸化物、その製造方法、並びに固体電解質型燃料電池
JP2000-236809 2000-08-04

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10336277A1 (de) * 2003-08-07 2005-03-24 Siemens Ag Maschineneinrichtung mit einer supraleitenden Wicklung und einer Thermosyphon-Kühlung derselben

Families Citing this family (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2005259518A (ja) * 2004-03-11 2005-09-22 Ngk Insulators Ltd 電気化学セル用アセンブリおよび電気化学セル
JP5085176B2 (ja) * 2006-04-07 2012-11-28 本田技研工業株式会社 排ガス浄化触媒および排ガス浄化装置
JP5313726B2 (ja) * 2009-03-10 2013-10-09 株式会社ノリタケカンパニーリミテド 固体酸化物形燃料電池および該電池用インターコネクタ
KR101104117B1 (ko) * 2010-05-11 2012-01-13 한국에너지기술연구원 원통형 고체산화물 연료전지의 공기극 집전체
CN106571481B (zh) * 2016-10-20 2019-08-27 湖北大学 一种锶钙共掺杂锰酸镧基钙钛矿材料及其在sofc中的应用
WO2019106994A1 (fr) * 2017-11-29 2019-06-06 株式会社村田製作所 Élément céramique

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0184665A1 (fr) * 1984-12-12 1986-06-18 DORNIER SYSTEM GmbH Céramique électriquement conductrice
JPH07267749A (ja) * 1994-03-28 1995-10-17 Ngk Insulators Ltd 多孔質焼結体及び固体電解質型燃料電池
JPH07277848A (ja) * 1994-04-13 1995-10-24 Ngk Insulators Ltd 多孔質焼結体、耐熱性電極及び固体電解質型燃料電池
JPH0864222A (ja) * 1994-08-26 1996-03-08 Mitsui Eng & Shipbuild Co Ltd 固体電解質型燃料電池用空気極及び空気極側集電板

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0184665A1 (fr) * 1984-12-12 1986-06-18 DORNIER SYSTEM GmbH Céramique électriquement conductrice
JPH07267749A (ja) * 1994-03-28 1995-10-17 Ngk Insulators Ltd 多孔質焼結体及び固体電解質型燃料電池
JPH07277848A (ja) * 1994-04-13 1995-10-24 Ngk Insulators Ltd 多孔質焼結体、耐熱性電極及び固体電解質型燃料電池
JPH0864222A (ja) * 1994-08-26 1996-03-08 Mitsui Eng & Shipbuild Co Ltd 固体電解質型燃料電池用空気極及び空気極側集電板

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10336277A1 (de) * 2003-08-07 2005-03-24 Siemens Ag Maschineneinrichtung mit einer supraleitenden Wicklung und einer Thermosyphon-Kühlung derselben

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JP2002053374A (ja) 2002-02-19

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