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WO2016148500A1 - Capteur de détection d'hydrogène pour détection d'hydrogène à large plage de concentration - Google Patents

Capteur de détection d'hydrogène pour détection d'hydrogène à large plage de concentration Download PDF

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Publication number
WO2016148500A1
WO2016148500A1 PCT/KR2016/002635 KR2016002635W WO2016148500A1 WO 2016148500 A1 WO2016148500 A1 WO 2016148500A1 KR 2016002635 W KR2016002635 W KR 2016002635W WO 2016148500 A1 WO2016148500 A1 WO 2016148500A1
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Prior art keywords
electrode layer
hydrogen
electrode
oxide
insulating layer
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Ceased
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PCT/KR2016/002635
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English (en)
Korean (ko)
Inventor
서형탁
이영안
노용규
에스카라누르 산카라
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Ajou University Industry Academic Cooperation Foundation
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Ajou University Industry Academic Cooperation Foundation
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Publication of WO2016148500A1 publication Critical patent/WO2016148500A1/fr
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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
    • G01N27/02—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating impedance
    • G01N27/22—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating impedance by investigating capacitance
    • G01N27/227—Sensors changing capacitance upon adsorption or absorption of fluid components, e.g. electrolyte-insulator-semiconductor sensors, MOS capacitors
    • 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
    • G01N27/02—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating impedance
    • G01N27/22—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating impedance by investigating capacitance

Definitions

  • the present invention relates to a hydrogen detection sensor that detects a wide range of concentrations of hydrogen, and can measure hydrogen by measuring capacitance changes caused by reaction with hydrogen.
  • Hydrogen sensors for hydrogen detection have been developed primarily to detect the presence of hydrogen. That is, the hydrogen sensor has been mainly developed in the direction of improving the detection sensitivity to detect the low concentration of hydrogen.
  • the most widely used hydrogen detection method is a method of measuring the electrical conductivity change of the palladium metal catalyst generated when the palladium (Pd) metal catalyst is exposed to hydrogen gas.
  • Hydrogen detection sensor comprises a first electrode layer disposed on the substrate surface; A second electrode layer disposed on the first electrode layer and including a catalyst metal capable of dissociating hydrogen molecules into hydrogen atoms; An insulating material disposed between the first electrode layer and the second electrode layer and having a lower surface in surface contact with the first electrode layer and an upper surface in surface contact with the second electrode layer and capable of reacting with a hydrogen atom to be reduced; A first insulating layer formed; And a capacitance meter electrically connected to the first electrode layer and the second electrode layer to measure a change in capacitance of the first insulating layer.
  • the catalytic metal is made of palladium (Pd), platinum (Pt), iridium (Ir), rhodium (Rh), silver (Ag), gold (Au), cobalt (Co) and alloys thereof It may include one or more selected from the group.
  • the insulating material is platinum oxide, palladium oxide, rhodium oxide, ruthenium oxide, beryllium oxide, manganese oxide ), Copper oxide, iron oxide, nickel oxide, cobalt oxide, cerium oxide, silver oxide, zirconium oxide And it may include one or more selected from the group consisting of boron nitride (boron nitride).
  • the hydrogen detection sensor may include: a third electrode layer disposed on the second electrode layer so as to be spaced apart from the second electrode layer, and including a catalyst metal capable of dissociating hydrogen molecules into hydrogen atoms; An insulating material disposed between the second electrode layer and the third electrode layer and having a lower surface in surface contact with the second electrode layer and an upper surface in surface contact with the third electrode layer and capable of reacting with a hydrogen atom to be reduced; A second insulating layer formed; And a connection wiring electrically connecting the first electrode layer and the third electrode layer.
  • Hydrogen detection sensor comprises a first electrode layer having a thin film electrode portion of a thin film structure formed on the surface of the substrate; An insulating layer disposed on the surface of the substrate to cover the surface of the thin film electrode part and formed of an insulating material capable of reducing by reacting with a hydrogen atom; A second electrode layer disposed on the surface of the substrate so as to cover the surface of the insulating layer, and having a hydrogen dissociation electrode portion made of a catalyst metal capable of dissociating hydrogen molecules into hydrogen atoms; And a capacitance meter electrically connected to the first electrode layer and the second electrode layer to measure a change in capacitance of the insulating layer.
  • the first electrode layer may further include a first through electrode part in contact with the thin film electrode part and penetrating the substrate.
  • the capacitance measuring part may be provided in the first through electrode part. Can be electrically connected.
  • the second electrode layer may further include a second through electrode part in contact with the hydrogen dissociation electrode part and penetrating the substrate, in which case, the capacitance measuring device may include the second through electrode part.
  • the second through electrode portion may be made of a metal different from the hydrogen dissociation electrode portion.
  • Hydrogen detection sensor comprises a first electrode layer disposed on the substrate surface; An insulating layer disposed on the first electrode layer and formed of an insulating material capable of reducing by reacting with a hydrogen atom; A second electrode layer disposed inside the insulating layer; A third electrode layer formed on the surface of the substrate to cover the surface of the insulating layer, the third electrode layer being in contact with the first electrode layer and including a catalyst metal capable of dissociating hydrogen molecules into hydrogen atoms; And a capacitance meter electrically connected to one of the first electrode layer and the third electrode layer and the second electrode layer to measure a change in capacitance of the insulating layer.
  • the second electrode layer may have a plate structure disposed in parallel with the first electrode layer.
  • hydrogen since hydrogen is detected using an electrode layer made of a catalyst metal capable of dissociating hydrogen molecules into hydrogen atoms and an insulating film made of a material capable of reacting with the hydrogen atoms, hydrogen can be detected at a high concentration.
  • the sensor may be configured to configure a plurality of capacitors connected in parallel, and the hydrogen concentration may be detected more precisely by detecting hydrogen through a change in capacitance of the insulating layer.
  • an external catalyst electrode layer By forming an external catalyst electrode layer so as to cover the surface of the insulating film, it is possible to prevent the insulating layer from being contaminated by external contaminants, thereby improving the life of the sensor.
  • FIG. 1 is a cross-sectional view for describing a hydrogen detection sensor according to an exemplary embodiment of the present invention.
  • FIG. 2 is a cross-sectional view for describing a hydrogen detection sensor according to another exemplary embodiment of the present invention.
  • FIG 3 is a cross-sectional view for describing a hydrogen detection sensor according to another exemplary embodiment of the present invention.
  • FIG. 4 is a cross-sectional view for describing a hydrogen detection sensor according to another exemplary embodiment of the present invention.
  • first and second may be used to describe various components, but the components should not be limited by the terms. The terms are used only for the purpose of distinguishing one component from another.
  • the first component may be referred to as the second component, and similarly, the second component may also be referred to as the first component.
  • FIG. 1 is a cross-sectional view for describing a hydrogen detection sensor according to an exemplary embodiment of the present invention.
  • the hydrogen detection sensor 100 may include a first electrode layer 110, an insulating layer 120, a second electrode layer 130, and a capacitance meter 140. Can be.
  • the first electrode layer 110 may have a thin film shape formed on the substrate 150 and may be formed of an electrically conductive material.
  • the first electrode layer 110 may be formed of a conductive metal, a conductive alloy, a conductive polymer, a conductive carbon-based material, or the like.
  • the first electrode layer 110 may be formed of a catalytic metal capable of dissociating hydrogen molecules into hydrogen atoms.
  • the catalyst metal includes, for example, palladium (Pd), platinum (Pt), iridium (Ir), rhodium (Rh), silver (Ag), gold (Au), cobalt (Co), alloys thereof, and the like. can do.
  • the material and structure of the substrate 150 are not particularly limited.
  • an insulating polymer substrate, a semiconductor substrate, or the like may be applied to the substrate 150 without limitation.
  • the insulating layer 120 may be formed on the first electrode layer 110 to be in surface contact with the first electrode layer 110.
  • the insulating layer 120 includes a lower surface in contact with the first electrode layer 110 and an upper surface in contact with the second electrode layer 130, and the first and second electrode layers 110. , 130) may have a structure having a constant thickness greater than. The thickness of the insulating layer 120 may be appropriately adjusted in consideration of the concentration range of hydrogen to be measured.
  • the insulating layer 120 may be formed of an insulating material that may be reduced by reacting with a hydrogen atom.
  • the insulating layer 120 may include platinum oxide, palladium oxide, rhodium oxide, ruthenium oxide, beryllium oxide, and manganese oxide. oxide, copper oxide, iron oxide, nickel oxide, cobalt oxide, cerium oxide, silver oxide, zirconium oxide ), Boron nitride and the like.
  • the second electrode layer 130 may be formed in a thin film form on the insulating layer 120 to be in surface contact with the upper surface of the insulating layer 120, and formed of a catalyst metal capable of dissociating hydrogen molecules into hydrogen atoms.
  • the catalyst metal includes, for example, palladium (Pd), platinum (Pt), iridium (Ir), rhodium (Rh), silver (Ag), gold (Au), cobalt (Co), alloys thereof, and the like. can do.
  • the second electrode layer 130 may be formed by coating catalytic metal nanoparticles on the insulating layer 120 to increase the contact area with hydrogen molecules and reduce the amount of catalyst metal used. .
  • the capacitance measuring unit 140 is electrically connected to the first electrode layer 110 and the second electrode layer 130 to measure the capacitance change of the insulating layer 120 caused by the reaction with hydrogen atoms. Can be.
  • the insulating layer 120 may have capacitance and electrical conductivity by reaction with hydrogen atoms. Will change.
  • the capacitance measuring unit 140 may determine the concentration of the external hydrogen gas by measuring a change in capacitance among changing properties of the insulating layer 120. On the other hand, the capacitance measuring unit 140 may further measure the change in the electrical resistance of the insulating layer 120.
  • FIG. 2 is a cross-sectional view for describing a hydrogen detection sensor according to another exemplary embodiment of the present invention.
  • the hydrogen detection sensor 200 may include a first electrode layer 210, a first insulating layer 220, a second electrode layer 230, and a second insulating layer 260.
  • the third electrode layer 270, the connection wiring 280, and the capacitance measuring instrument 240 may be included.
  • the first electrode layer 210, the first insulating layer 220, the second electrode layer 230, and the capacitance meter 250 may include the first electrode layer 110 of the hydrogen detection sensor 100 described with reference to FIG. 1, Since the insulating layer 120, the second electrode layer 130, and the capacitance meter 140 are substantially the same, detailed descriptions thereof will be omitted.
  • the second insulating layer 260 may be formed on the second electrode layer 230 to be in surface contact with the second electrode layer 230.
  • the second insulating layer 260 has a lower surface in contact with the second electrode layer 230 and an upper surface in contact with the third electrode layer 270, and the first to third electrode layers. It may have a structure having a constant thickness greater than (210, 230, 270).
  • the thickness of the second insulating layer 260 may be the same as or different from the thickness of the first insulating layer 220, and the thickness of the first and second insulating layers 220 and 260 may be measured.
  • the concentration range of the hydrogen gas can be adjusted appropriately.
  • the second insulating layer 260 may be formed of an insulating material that can be reduced by reacting with a hydrogen atom.
  • the second insulating layer 260 may include platinum oxide, palladium oxide, rhodium oxide, ruthenium oxide, beryllium oxide, and manganese oxide. (manganese oxide, copper oxide, iron oxide, nickel oxide, cobalt oxide, cerium oxide, silver oxide, zirconium oxide ( It may be formed of one or more materials selected from zirconium oxide, boron nitride and the like.
  • the second insulating layer 260 may be formed of the same material as the first insulating layer 220 or may be formed of a material different from that of the first insulating layer 220.
  • the third electrode layer 270 may be formed in a thin film form on the second insulating layer 260 to be in surface contact with the upper surface of the second insulating layer 260, and may dissociate hydrogen molecules into hydrogen atoms. It may be formed of a catalytic metal.
  • the catalyst metal includes, for example, palladium (Pd), platinum (Pt), iridium (Ir), rhodium (Rh), silver (Ag), gold (Au), cobalt (Co), alloys thereof, and the like. can do.
  • the third electrode layer 270 may be formed by applying catalytic metal nanoparticles to increase the contact area with hydrogen molecules and reduce the amount of catalyst metal used.
  • the connection wiring 280 may be formed of a conductive material and may electrically connect the first electrode layer 210 and the third electrode layer 270. As such, when the first electrode layer 210 and the third electrode layer 270 are electrically connected to each other through the connection wiring 280, the first electrode layer 210, the first insulating layer 220, and the The first capacitor defined by the second electrode layer 230 and the second capacitor defined by the second electrode layer 230, the second insulating layer 260, and the third electrode layer 270 may be connected in parallel. have. In this case, when the first capacitor and the second capacitor are connected in parallel using the connection wiring 280, the capacitance generated in the first insulating layer 220 and the second insulating layer 260. The change of can be measured more sensitively, and as a result, the concentration of hydrogen gas can be measured more precisely.
  • FIG 3 is a cross-sectional view for describing a hydrogen detection sensor according to another exemplary embodiment of the present invention.
  • the hydrogen detection sensor 300 includes a first electrode layer 310, an insulating layer 320, a second electrode layer 330, and a capacitance meter 340. can do.
  • the first electrode layer 310 may have a thin film electrode part 311 having a thin film shape formed on the substrate 350 and the thin film electrode part 311 from an external circuit, for example, the capacitance measuring device ( It may include a first through electrode portion 312 formed to penetrate the substrate 350 to connect to the 340.
  • the thin film electrode part 311 and the first through electrode part 312 may be formed of an electrically conductive material. Meanwhile, the thin film electrode part 311 and the first through electrode part 312 may be formed of the same material or may be formed of different materials.
  • the insulating layer 320 may be formed on the substrate 350 to cover the entire surface of the thin film electrode part 311 of the first electrode layer 310.
  • the insulating layer 320 may be formed of an insulating material that may be reduced by reacting with a hydrogen atom.
  • the insulating layer 320 may include platinum oxide, palladium oxide, rhodium oxide, ruthenium oxide, beryllium oxide, and manganese oxide. oxide, copper oxide, iron oxide, nickel oxide, cobalt oxide, cerium oxide, silver oxide, zirconium oxide ), Boron nitride and the like.
  • the second electrode layer 330 may include a hydrogen dissociation electrode 331 formed on the substrate 350 to cover the entire surface of the insulating layer 320.
  • the hydrogen dissociation electrode unit 331 may be formed of a catalyst metal capable of dissociating hydrogen molecules into hydrogen atoms.
  • the catalyst metal includes, for example, palladium (Pd), platinum (Pt), iridium (Ir), rhodium (Rh), silver (Ag), gold (Au), cobalt (Co), alloys thereof, and the like. can do.
  • the hydrogen dissociation electrode unit 331 is formed by applying catalytic metal nanoparticles on the surface of the insulating layer 320 in order to increase the contact area with hydrogen molecules and reduce the amount of catalyst metal used. Can be.
  • the second electrode layer 330 may be electrically connected to an external circuit, for example, the capacitance meter 340 through the hydrogen dissociation electrode 332, but may be electrically connected to the capacitance meter 340. It may further include a second through electrode portion 332 penetrating the substrate 350 to be connected.
  • the second through electrode part 332 may be formed of the same material as the hydrogen dissociation electrode part 331 but may be formed of a material different from that of the hydrogen dissociation electrode part 331.
  • the hydrogen dissociation electrode unit 331 may be formed of the catalyst metal
  • the second through electrode unit 332 may be formed of a metal material different from that of the catalyst metal.
  • the capacitance measuring instrument 340 is electrically connected to the first electrode layer 310 and the second electrode layer 330 to measure the capacitance change of the insulating layer 320 caused by the reaction with hydrogen atoms. Can be.
  • the capacitance measuring device 340 may be electrically connected to the first electrode layer 310 through the first through electrode part 312, and the hydrogen dissociation electrode part 331 and the second electrode may be electrically connected to the first electrode layer 310.
  • the second electrode layer 330 may be electrically connected to one of the through electrode portions 332.
  • the hydrogen dissociation electrode 331 made of the catalyst metal is hydrogen. Since it is possible to block other contaminating gases except for preventing the insulating layer 320 from being contaminated by an external contaminating gas to improve the life of the hydrogen detection sensor 300.
  • the first electrode layer 310 and the second electrode layer ( 330 may be electrically insulated.
  • FIG. 4 is a cross-sectional view for describing a hydrogen detection sensor according to another exemplary embodiment of the present invention.
  • the hydrogen detection sensor 400 may include a first electrode layer 410, an insulating layer 420, a second electrode layer 430, a third electrode layer 450, and an electrostatic discharge. Capacity meter 440 may be included.
  • the first electrode layer 410 may have a thin film shape formed on the substrate 450 and may be formed of an electrically conductive material.
  • the first electrode layer 410 may be formed of a conductive metal, a conductive alloy, a conductive polymer, a conductive carbon-based material, or the like.
  • the first electrode layer 410 may be formed of a catalytic metal capable of dissociating hydrogen molecules into hydrogen atoms.
  • the catalyst metal includes, for example, palladium (Pd), platinum (Pt), iridium (Ir), rhodium (Rh), silver (Ag), gold (Au), cobalt (Co), alloys thereof, and the like. can do.
  • the insulating layer 420 may be formed on the first electrode layer 410 to be in surface contact with the first electrode layer 410.
  • the insulating layer 420 may have a lower surface in contact with the first electrode layer 410 and an upper surface in contact with the second electrode layer 430, and may have a structure having a predetermined thickness. .
  • the thickness of the insulating layer 420 may be appropriately adjusted in consideration of the concentration range of hydrogen to be measured.
  • the insulating layer 420 may be formed of an insulating material that may be reduced by reacting with a hydrogen atom.
  • the insulating layer 120 may include platinum oxide, palladium oxide, rhodium oxide, ruthenium oxide, beryllium oxide, and manganese oxide. oxide, copper oxide, iron oxide, nickel oxide, cobalt oxide, cerium oxide, silver oxide, zirconium oxide ), Boron nitride and the like.
  • the second electrode layer 430 may be disposed in the insulating layer 420.
  • the second electrode layer 430 may have a plate structure having a predetermined thickness, and may be disposed in parallel with the first electrode layer 410 inside the insulating layer 420.
  • the material of the second electrode layer 430 is not particularly limited and may be formed of an electrically conductive material.
  • the formation method of a said 2nd electrode layer is not specifically limited. For example, a part of the insulating layer 420 is formed on the first electrode layer 410, and then a conductive material is applied thereon to form the second electrode layer 430, and then the second electrode layer 430.
  • the second electrode layer 430 may be formed inside the insulating layer 420 by completing the insulating layer 420 by applying an insulating material on a portion of the insulating layer 420 on which is formed.
  • the third electrode layer 450 may be formed on the surface of the insulating layer 420 so as to cover the entire surface of the insulating layer 420, and contact the first electrode layer 410 at a lower end thereof to contact the first electrode layer 410. It may be electrically connected to the electrode layer 410.
  • the third electrode layer 450 may be formed of a catalyst metal capable of dissociating hydrogen molecules into hydrogen atoms.
  • the catalyst metal includes, for example, palladium (Pd), platinum (Pt), iridium (Ir), rhodium (Rh), silver (Ag), gold (Au), cobalt (Co), alloys thereof, and the like. can do.
  • the third electrode layer 270 may be formed by applying catalytic metal nanoparticles to increase the contact area with hydrogen molecules and reduce the amount of catalyst metal used.
  • the third electrode layer 450 when the third electrode layer 450 is electrically connected to the first electrode layer 410 and covers the entire surface of the insulating layer 420, the capacitance of the insulating layer 420 may be reduced. Not only can the change be more sensitively measured, but the insulating layer 420 can be prevented from being contaminated by external polluting gases. Specifically, when the third electrode layer 450 is formed to be electrically connected to the first electrode layer 210, the first electrode layer 410, the second electrode layer 430, and the insulating layer disposed therebetween.
  • a first capacitor defined by a portion of 420 and a second capacitor defined by the second electrode layer 430 and the third electrode layer 450 and a portion of the insulating layer 420 positioned therebetween are Since connected in parallel, it is possible to more sensitively measure the change in capacitance generated in the entire insulating layer 420. Since the third electrode layer 450 covers the entire surface of the insulating layer 420, the insulating layer 420 may be protected from external contaminants by the third electrode layer 450.

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Abstract

L'invention concerne un capteur de détection d'hydrogène. Le capteur de détection d'hydrogène comprend : une première couche d'électrode disposée sur la surface d'un substrat ; une seconde couche d'électrode disposée sur la partie supérieure de la première couche d'électrode, la seconde couche d'électrode comprenant un catalyseur métallique apte à dissocier des molécules d'hydrogène en atomes d'hydrogène ; une couche isolante disposée entre la première couche d'électrode et la seconde couche d'électrode, la couche isolante étant formée d'un matériau isolant apte à être réduit par réaction avec les atomes d'hydrogène ; et un dispositif de mesure de capacité pour mesurer des variations de capacité de la couche isolante.
PCT/KR2016/002635 2015-03-17 2016-03-16 Capteur de détection d'hydrogène pour détection d'hydrogène à large plage de concentration Ceased WO2016148500A1 (fr)

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KR10-2015-0036631 2015-03-17
KR1020150036631A KR101550173B1 (ko) 2015-03-17 2015-03-17 광범위 농도의 수소를 검출하는 수소 검출 센서

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KR101679778B1 (ko) * 2015-04-15 2016-11-25 포항공과대학교 산학협력단 가역적 수소저장소자 및 그 사용방법
JP2024085275A (ja) * 2022-12-14 2024-06-26 株式会社東芝 センサ

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KR20060088700A (ko) * 2005-02-02 2006-08-07 엘지전자 주식회사 정전용량 변화를 이용한 수소센서 및 그 제조방법
KR20060111296A (ko) * 2005-04-22 2006-10-27 엘지전자 주식회사 수소 센서 및 그 제조 방법
KR101052164B1 (ko) * 2008-11-27 2011-07-26 한국원자력연구원 방사선 및 가스 동시 측정센서 및 이의 제조방법

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