WO2018003308A1 - 電気化学ガスセンサ - Google Patents
電気化学ガスセンサ Download PDFInfo
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- WO2018003308A1 WO2018003308A1 PCT/JP2017/017821 JP2017017821W WO2018003308A1 WO 2018003308 A1 WO2018003308 A1 WO 2018003308A1 JP 2017017821 W JP2017017821 W JP 2017017821W WO 2018003308 A1 WO2018003308 A1 WO 2018003308A1
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- lid
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- gas diffusion
- mea
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/403—Cells and electrode assemblies
- G01N27/406—Cells and probes with solid electrolytes
- G01N27/407—Cells and probes with solid electrolytes for investigating or analysing gases
-
- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/403—Cells and electrode assemblies
- G01N27/406—Cells and probes with solid electrolytes
- G01N27/407—Cells and probes with solid electrolytes for investigating or analysing gases
- G01N27/4071—Cells and probes with solid electrolytes for investigating or analysing gases using sensor elements of laminated structure
- G01N27/4072—Cells and probes with solid electrolytes for investigating or analysing gases using sensor elements of laminated structure characterized by the diffusion barrier
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/403—Cells and electrode assemblies
- G01N27/404—Cells with anode, cathode and cell electrolyte on the same side of a permeable membrane which separates them from the sample fluid, e.g. Clark-type oxygen sensors
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/403—Cells and electrode assemblies
- G01N27/406—Cells and probes with solid electrolytes
- G01N27/407—Cells and probes with solid electrolytes for investigating or analysing gases
- G01N27/4071—Cells and probes with solid electrolytes for investigating or analysing gases using sensor elements of laminated structure
-
- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/416—Systems
-
- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/416—Systems
- G01N27/4162—Systems investigating the composition of gases, by the influence exerted on ionic conductivity in a liquid
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/416—Systems
- G01N27/417—Systems using cells, i.e. more than one cell and probes with solid electrolytes
Definitions
- the present invention relates to a housing structure for an electrochemical gas sensor.
- Patent Document 1 JP5693,496B
- Patent Document 2 WO 01 / 014864A
- the MEA that constitutes the gas sensor main body includes a detection electrode and a counter electrode on both surfaces of a proton conductor film or a liquid retaining sheet that holds an electrolyte, an ionic fluid, or the like. Then, the current or electromotive force flowing between the electrodes generated by contact with the gas becomes the output.
- the MEA is sandwiched between a pair of breathable conductive films (conductive gas diffusion films), supplied with an atmosphere to be detected from the conductive film on the detection electrode side, and supplied with oxygen from the conductive film on the counter electrode side.
- the generated water vapor is discharged from the counter electrode (Patent Document 1).
- Patent Document 1 proposes a structure similar to that of a button-type battery, and a conductive film and an MEA are disposed between two metal plates insulated by a gasket, and two metal sheets are formed. Secure the plate with caulking. Electrical contact from the MEA to the two metal plates is obtained by the caulking pressure.
- Patent Document 2 a pair of housings with dents are stacked so that the dents face each other, and the MEA is disposed in the dents.
- the recess is also used as a reservoir for the liquid electrolyte, and the electrode is exposed through a hole or the like of the housing so that it can be connected to the outside.
- This invention is to provide an electrochemical gas sensor that can be easily miniaturized, has small performance variations, and can be easily mounted on a substrate.
- the electrochemical gas sensor of the present invention is A ceramic housing having a plate shape and a recess;
- An MEA comprising an ion conductive film, a first electrode on the surface of the ion conductive film, and a second electrode on the back surface;
- a metal lid fixed to the housing so as to cover the recess,
- the housing includes a first electrical wiring extending from the bottom surface of the recess to the bottom surface of the housing, and a second electrical wiring extending from the top surface surrounding the recess to the bottom surface of the housing;
- the first conductive gas diffusion film is disposed between the MEA and the bottom surface of the recess, and is electrically connected to the first electrical wiring,
- a second conductive gas diffusion film is disposed between the MEA and the lid and electrically connected to the lid;
- the lid is fixed to the top surface and electrically connected to the second electrical wiring; By the lid, the second conductive gas diffusion film is pressed
- the electrochemical gas sensor can be miniaturized.
- the lid causes the first and second conductive gas diffusion films and the MEA to be pressed toward the bottom surface of the recess, and the electrical path from the MEA to the lid through the second conductive gas diffusion film and the MEA to the first An electrical path to the first electrical wiring is obtained through one conductive gas diffusion film.
- the second electrical wiring leads to the bottom surface of the housing, and the first electrical wiring also extends to the bottom surface of the housing. Therefore, the two electrodes of the gas sensor can be connected to the peripheral circuit on the bottom surface of the housing. In this specification, the direction is shown with the lid up and the bottom of the dent down.
- a metal layer is provided on the top surface, and the lid is welded to the metal layer. Since the lid is welded to the metal layer, the lid and the housing can be easily fixed, and the lid and the metal layer can be securely and airtightly connected.
- the lid includes a hole as the gas introduction portion, and the bottom surface of the housing is airtight. Since the lid is a metal, it is possible to accurately provide a small-diameter gas introduction hole and to maintain a constant air permeability into the gas sensor. Further, since the gas introduction hole is provided in the lid, the bottom surface of the housing is made airtight.
- a conductive and sheet-like gas adsorption filter is provided between the second conductive gas diffusion film and the lid.
- Some activated carbons are conductive, and gas adsorbents such as silica gel, zeolite, and mesoporous silica can be imparted with conductivity by mixing conductive particles such as carbon black. Therefore, it is possible to secure a conductive path from the second conductive gas diffusion film to the lid through the gas adsorption filter.
- the gas adsorption filter since the gas adsorption filter only needs to process a small amount of gas diffused from the gas introduction hole of the lid, the life of the filter can be extended.
- the MEA, the first conductive gas diffusion film, the second conductive gas diffusion film, the recess, the housing, and the lid are quadrangular, for example, rectangular or square in plan view. Since a quadrangular MEA is used instead of the circular MEA as in Patent Document 1, loss can be reduced when the MEA is punched from the original sheet. As the MEA is squared, the housing, lid, dent, and first and second conductive gas diffusion films are also squared.
- the recess includes a bottom surface, a first wall surrounding the bottom surface, a flat surface on the top of the first wall, and a second wall surrounding the flat surface, and the top of the second wall There is a top surface,
- the first conductive gas diffusion film is in contact with the bottom surface of the recess and surrounded by the first wall;
- the second conductive gas diffusion film is surrounded by a second wall;
- An end of the MEA or an end of the second conductive gas diffusion film is located on the flat surface.
- the conductive gas diffusion film is compressed by the pressure from the lid, and the pressure includes contact between the first conductive gas diffusion film and the MEA, and the second conductive gas diffusion film, the MEA, and the first electric wiring. There is an action to ensure contact with. If a flat surface is provided between the bottom surface and the top surface of the recess, and the recess is divided into a portion from the top surface to the flat surface and a portion from the flat surface to the bottom surface along the depth direction, The thickness of the first conductive gas diffusion film and the thickness of the first conductive gas diffusion film can be regulated. In addition, since the end of the MEA or the end of the second conductive gas diffusion film is located on the flat surface, the two conductive gas diffusion films do not contact each other, and between the upper and lower sides of the flat surface. With this, the atmosphere can be shut off.
- Sectional view of the electrochemical gas sensor of the example Plan view of the electrochemical gas sensor of the example Plan view of the electrochemical gas sensor of the embodiment with the lid removed Sectional drawing of housing of electrochemical gas sensor of embodiment
- the electrochemical gas sensor 2 includes a ceramic housing 4, an MEA 6, conductive gas diffusion films 8 and 10 above and below the MEA 6, and a metal lid 12. These members 4 to 12 are rectangular to square in plan view, and the MEA 6 and the conductive gas diffusion films 8 and 10 are accommodated in the recess 13 of the housing 4.
- the housing 4 includes a rectangular to square recess 13 in plan view, 14 is a bottom surface of the recess 13, 15 is an intermediate flat surface, and surrounds the bottom surface 14, and 25 is a top surface and surrounds the flat surface 15. Between the top surface 25 and the flat surface 15, for example, there is a vertical wall surface 17, and between the flat surface 15 and the bottom surface 14, for example, there is a vertical wall surface 18.
- the metal layer 16 may be formed by firing a metal together with the ceramic material of the housing 4 or fixing a metal plate to the top surface 25 by brazing or the like. The metal layer 16 is connected to the electrical wiring 21 on the bottom surface 19 of the housing 4 via the electrical wiring 20.
- a wiring 22 is provided on the entire surface or a part of the bottom surface 14 of the recess 13 and is drawn out to the bottom surface 19 of the housing 4 via the wirings 23 and 24.
- the wirings 20 to 24 are made by firing a metal together with the ceramic material of the housing 4. Instead of providing the wirings 20 and 23 on the end surface of the housing 4, a conductive airtight through hole may be provided in the housing 4.
- the lid 12 is provided with one or a plurality of gas introduction holes 26, and by making the size of the gas introduction holes 26 constant, the air permeability to the inside of the gas sensor 2 is made constant. Since the hole is formed in the metal, the gas introduction hole 26 having a certain size can be formed. Instead of providing the gas introduction hole in the lid 12, the layer from the bottom surface 19 of the housing 4 to the bottom surface 14 of the recess 13 may be made of breathable ceramics.
- the MEA 6 is provided with a detection electrode 35 on the proton conductor film 34 and a counter electrode 36 on the lower part.
- a sheet holding an electrolytic solution or an ionic fluid may be used instead of the proton conductor film 34.
- the MEA 6 is the most expensive member in the gas sensor 2, and the MEA 6 is manufactured by punching from the original sheet of the MEA 6, and no loss due to punching occurs in the rectangular to square MEA 6.
- the conductive gas diffusion films 8 and 10 are air permeable sheets having conductive particles such as carbon black and carbon fiber, and do not require high conductivity.
- the diffusion films 8 and 10 may be hydrophobized by adding fibers such as PTFE.
- fibers such as PTFE.
- hydrophilic fibers such as polyamide, methylcellulose, and polyvinyl alcohol are mixed to provide moisture conditioning, and the humidity dependence of the gas sensor 2 is increased. Make it smaller.
- a filter which is a sheet of activated carbon having air permeability and conductivity, which is disposed between the lid 2 and the first conductive film 8 and electrically connects them.
- a sheet formed by mixing conductive particles with another adsorbent such as zeolite, silica gel, or mesoporous silica and then molding with a fibrous binder can also be used.
- the housing 4 includes three layers 30 to 32.
- the wirings 21, 22, and 24 are formed on both sides of the layer 30, and the metal layer 16 is formed on the top surface 25 of the layer 32. It is manufactured by stacking layers 30 to 32 and firing.
- the wirings 20 and 23 may be formed simultaneously with the layers 30 to 32 and fired at the same time, or may be formed after the layers 30 to 32 are fired.
- the conductive gas diffusion films 8 and 10 are stacked above and below the MEA 6, and for example, the conductive gas diffusion film 10 is disposed on the bottom surface 14 of the recess 13. Either one of the ends of the MEA 6 and the conductive gas diffusion film 8 is supported by the flat surface 15 to prevent the conductive gas diffusion films 8 and 10 from coming into contact with each other, and above and below the flat surface 15. Separate the atmosphere.
- the filter 28 is overlapped on the gas diffusion film 8, the recess 13 is covered with the lid 12, and the lid 12 is welded to the metal layer 16 by seam welding.
- Seam welding is used for sealing an IC chip to a ceramic package, and the lid 12 can be fixed to the housing 4 easily and airtightly. Note that, instead of seam welding, bonding with a conductive adhesive is also possible.
- the filter 12, the conductive gas diffusion film 8, the MEA 6, and the conductive gas diffusion film 10 are pressed toward the bottom surface 14 of the recess 13 by the lid 12, so that these members are electrically connected and the position is also constant.
- the conductive gas diffusion films 8 and 10 are thinned by pressurization, and the thickness after pressurization is determined by the height of the wall surface 18 in the conductive gas diffusion film 10, and the height of the wall surface 17 in the conductive gas diffusion film 8. It depends on. Further, since the ends of the MEA 6 and the conductive gas diffusion film 8 are on the flat surface 15, the conductive gas diffusion films 8 and 10 do not contact each other. Further, the gap between the wall surface 18 and the conductive gas diffusion film 10 is covered by the MEA 6 and the conductive gas diffusion film 8 and restricts the atmosphere on the detection electrode side from flowing to the counter electrode side.
- the detection electrode and the counter electrode of the MEA 6 are connected to the wirings 21 and 24 on the bottom surface of the housing 4, and the gas sensor 2 can be mounted on a substrate such as a printed circuit board by reflow soldering, conductive adhesive, or the like.
- FIG. 6 shows the electrochemical gas sensor 42 of the first modified example, which is the same as the embodiment of FIGS.
- a filter 48 made of a gas adsorbent is disposed above the gas introduction hole 26 of the lid 12. Since the gas before the air flow is reduced by the gas introduction hole 26 is processed, a larger filter 48 is required as compared with the filter 28. *
- FIG. 7 shows an electrochemical gas sensor 52 of a second modification, which is the same as the embodiment of FIGS.
- the MEA 6 and the gas diffusion films 8 and 10 and the filter 28 are not formed using the two-step recess 13 having the flat surface 15 in the middle in FIGS. To accommodate.
- Reference numeral 57 denotes a wall surface of the recess 53.
- Electrochemical gas sensor 4 Housing 6 MEA 8, 10 Conductive gas diffusion film 12 Lid 13 Recess 14 Recess bottom 15 Flat surface 16 Metal layer 17, 18 Wall 19 Housing bottom 20-24 Wiring 25 Top 26 Gas introduction hole 28, 48 Filter 30-32 Layer 34 Proton conductor film 35 Detection electrode 36 Counter electrode 42, 52 Electrochemical gas sensor 53 Recess 57 Wall surface
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Abstract
Description
板状でかつ凹みを有するセラミックスのハウジングと、
イオン導電性膜と、イオン導電性膜の表面の第1の電極と、裏面の第2の電極とを備えているMEAと、
第1の導電性ガス拡散膜と、第2の導電性ガス拡散膜と、
前記凹みを覆うように、前記ハウジングに固着されている、金属のリッドとを有し、
前記ハウジングは、前記凹みの底面からハウジングの底面へ延びる第1の電気配線と、前記凹みを取り囲む頂面から、ハウジングの底面へ延びる第2の電気配線とを備え、
第1の導電性ガス拡散膜は、前記MEAと前記凹みの底面との間に配置され、かつ前記第1の電気配線に電気的に接続され、
第2の導電性ガス拡散膜は、前記MEAと前記リッドとの間に配置され、かつ前記リッドに電気的に接続され、
前記リッドは、前記頂面に固着されると共に、前記第2の電気配線に電気的に接続され、
前記リッドにより、前記第2の導電性ガス拡散膜が前記MEA側へ押圧され、
前記リッドもしくは前記ハウジングの底面に、ガス導入部が設けられている。
前記第1の導電性ガス拡散膜は、凹みの底面に接触し、かつ第1の壁に囲まれ、
前記第2の導電性ガス拡散膜は第2の壁に囲まれ、
前記MEAの端部もしくは前記第2の導電性ガス拡散膜の端部が、前記平坦面上に位置する。
8,10 導電性ガス拡散膜 12 リッド 13 凹み
14 凹みの底面 15 平坦面 16 金属層
17,18 壁面 19 ハウジングの底面 20~24 配線
25 頂面 26 ガス導入孔 28,48 フィルタ
30~32 層 34 プロトン導電体膜 35 検出極
36 対極 42,52 電気化学ガスセンサ 53 凹み
57 壁面
Claims (6)
- 板状でかつ凹みを有するセラミックスのハウジングと、
イオン導電性膜と、イオン導電性膜の表面の第1の電極と、裏面の第2の電極とを備えているMEAと、
第1の導電性ガス拡散膜と、第2の導電性ガス拡散膜と、
前記凹みを覆うように、前記ハウジングに固着されている、金属のリッドとを有し、
前記ハウジングは、前記凹みの底面からハウジングの底面へ延びる第1の電気配線と、前記凹みを取り囲む頂面から、ハウジングの底面へ延びる第2の電気配線とを備え、
第1の導電性ガス拡散膜は、前記MEAと前記凹みの底面との間に配置され、かつ前記第1の電気配線に電気的に接続され、
第2の導電性ガス拡散膜は、前記MEAと前記リッドとの間に配置され、かつ前記リッドに電気的に接続され、
前記リッドは、前記頂面に固着されると共に、前記第2の電気配線に電気的に接続され、
前記リッドにより、前記第2の導電性ガス拡散膜が前記MEA側へ押圧され、
前記リッドもしくは前記ハウジングの底面に、ガス導入部が設けられている、電気化学ガスセンサ。 - 前記頂面上に金属層が設けられ、かつ前記リッドが前記金属層に溶接されていることを特徴とする、請求項1の電気化学ガスセンサ。
- 前記リッドは、前記ガス導入部として、孔を備え、かつ前記ハウジングの底面は気密であることを特徴とする、請求項1または2の電気化学ガスセンサ。
- 前記第2の導電性ガス拡散膜と前記リッドとの間に、導電性でかつシート状のガス吸着フィルタが設けられていることを特徴とする、請求項1~3のいずれかの電気化学ガスセンサ。
- 前記MEA、第1の導電性ガス拡散膜、第2の導電性ガス拡散膜、前記凹み、前記ハウジング、及び前記リッドが、平面視で四角形であることを特徴とする、請求項1~4のいずれかの電気化学ガスセンサ。
- 前記凹みは、底面と、底面を取り囲む第1の壁と、第1の壁の上部の平坦面と、平坦面を取り囲む第2の壁とを備え、第2の壁の上部に前記頂面が存在し、
前記第1の導電性ガス拡散膜は、凹みの底面に接触し、かつ第1の壁に囲まれ、
前記第2の導電性ガス拡散膜は第2の壁に囲まれ、
前記MEAの端部もしくは前記第2の導電性ガス拡散膜の端部が前記平坦面上に位置することを特徴とする、請求項1~5のいずれかの電気化学ガスセンサ。
Priority Applications (6)
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JP2018524938A JP6532118B2 (ja) | 2016-07-01 | 2017-05-11 | 電気化学ガスセンサ |
CN201780038652.6A CN109313159B (zh) | 2016-07-01 | 2017-05-11 | 电化学气体传感器 |
KR1020187036488A KR102173077B1 (ko) | 2016-07-01 | 2017-05-11 | 전기화학 가스센서 |
US16/308,523 US10976280B2 (en) | 2016-07-01 | 2017-05-11 | Electrochemical gas sensor |
GB1820273.9A GB2566198B (en) | 2016-07-01 | 2017-05-11 | Electrochemical gas sensor |
DE112017003327.6T DE112017003327T5 (de) | 2016-07-01 | 2017-05-11 | Elektrochemischer Gassensor |
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JP2016131346 | 2016-07-01 | ||
JP2016-131346 | 2016-07-01 |
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JP (1) | JP6532118B2 (ja) |
KR (1) | KR102173077B1 (ja) |
CN (1) | CN109313159B (ja) |
DE (1) | DE112017003327T5 (ja) |
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JP2019120655A (ja) * | 2018-01-11 | 2019-07-22 | フィガロ技研株式会社 | Co検出装置の温度補正係数の設定方法 |
WO2022181249A1 (ja) * | 2021-02-26 | 2022-09-01 | パナソニックIpマネジメント株式会社 | 電気化学式ガスセンサおよび電気化学式ガスセンサの製造方法 |
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KR20210103847A (ko) | 2020-02-14 | 2021-08-24 | 한양대학교 산학협력단 | 반고체 전해질 및 그 제조방법, 그리고 이를 포함하는 가스센서 |
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CN109313159A (zh) | 2019-02-05 |
GB201820273D0 (en) | 2019-01-30 |
GB2566198A (en) | 2019-03-06 |
JPWO2018003308A1 (ja) | 2018-10-25 |
GB2566198B (en) | 2021-10-06 |
US10976280B2 (en) | 2021-04-13 |
KR20190008345A (ko) | 2019-01-23 |
CN109313159B (zh) | 2020-12-01 |
JP6532118B2 (ja) | 2019-06-19 |
KR102173077B1 (ko) | 2020-11-02 |
US20190339226A1 (en) | 2019-11-07 |
DE112017003327T5 (de) | 2019-03-28 |
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