US20150004070A1 - Ozone generation apparatus - Google Patents

Ozone generation apparatus Download PDF

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Publication number
US20150004070A1
US20150004070A1 US14/487,445 US201414487445A US2015004070A1 US 20150004070 A1 US20150004070 A1 US 20150004070A1 US 201414487445 A US201414487445 A US 201414487445A US 2015004070 A1 US2015004070 A1 US 2015004070A1
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United States
Prior art keywords
electrode
ozone generation
dielectric
generation apparatus
discharge gap
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Abandoned
Application number
US14/487,445
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English (en)
Inventor
Takaaki Murata
Yuji Okita
Kiyoyuki Amemori
Kie Kubo
Ryutaro Makise
Kazuhiko Noda
Ryouichi Takahashi
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Toshiba Corp
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Toshiba Corp
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Publication date
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Assigned to KABUSHIKI KAISHA TOSHIBA reassignment KABUSHIKI KAISHA TOSHIBA ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: TAKAHASHI, RYOICHI, MURATA, TAKAAKI, KUBO, KIE, MAKISE, RYUTARO, AMEMORI, KIYOYUKI, NODA, KAZUHIKO, OKITA, YUJI
Publication of US20150004070A1 publication Critical patent/US20150004070A1/en
Priority to US15/136,286 priority Critical patent/US10759661B2/en
Abandoned legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B13/00—Oxygen; Ozone; Oxides or hydroxides in general
    • C01B13/10—Preparation of ozone
    • C01B13/11—Preparation of ozone by electric discharge
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B13/00—Oxygen; Ozone; Oxides or hydroxides in general
    • C01B13/10—Preparation of ozone
    • C01B13/11—Preparation of ozone by electric discharge
    • C01B13/115—Preparation of ozone by electric discharge characterised by the electrical circuits producing the electrical discharge
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J19/087—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J19/088—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0809—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes employing two or more electrodes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2201/00—Preparation of ozone by electrical discharge
    • C01B2201/20—Electrodes used for obtaining electrical discharge
    • C01B2201/22—Constructional details of the electrodes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2201/00—Preparation of ozone by electrical discharge
    • C01B2201/30—Dielectrics used in the electrical dischargers
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2201/00—Preparation of ozone by electrical discharge
    • C01B2201/30—Dielectrics used in the electrical dischargers
    • C01B2201/32—Constructional details of the dielectrics
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2201/00—Preparation of ozone by electrical discharge
    • C01B2201/60—Feed streams for electrical dischargers
    • C01B2201/62—Air
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2201/00—Preparation of ozone by electrical discharge
    • C01B2201/70—Cooling of the discharger; Means for making cooling unnecessary
    • C01B2201/74—Cooling of the discharger; Means for making cooling unnecessary by liquid
    • C01B2201/76—Water

Definitions

  • Embodiments of the present invention relate to an ozone generation apparatus.
  • a general ozone generation apparatus includes a dielectric electrode and a metal electrode disposed in an airtight vessel.
  • a ring-shaped spacer is inserted between the dielectric electrode and the metal electrode to form a discharge gap.
  • a conductive film is provided on an inner circumference face of the dielectric electrode.
  • a raw material gas introduced from a gas inlet into the airtight vessel flows through the discharge gap between the dielectric electrode and the metal electrode, and flows out from a gas outlet.
  • dielectric barrier discharge is formed in the discharge gap and ozone is generated.
  • dielectric barrier discharge is called simply barrier discharge or silent discharge sometimes.
  • Heat generated by the dielectric barrier discharge is cooled by cooling water supplied into a cooling water flow path formed by the metal electrode and the airtight vessel. As a result, temperature rise of gas in the discharge gap is suppressed and ozone is obtained efficiently.
  • a discharge gap length d is set to be in the range of 0.6 to 1.3 mm.
  • a gas pressure p of air which is raw material gas is set to be in the range of 0.17 to 0.28 MPa (absolute pressure).
  • the product of the gas pressure p of the raw material gas and the discharge gap length d is generally called pd product.
  • the law of discharge similarity holds true by making the pd product constant. This is because the pd product represents the number of gas molecules in the discharge gap.
  • Multiplication of electrons travelling in the discharge gap is represented by the product of the ionization coefficient ⁇ of the gas and the discharge gap length d.
  • the ad product is represented by
  • ⁇ /p represents ionization caused by single collision
  • the pd product represents the number of molecules contained in the discharge gap. This is the reason why the famous Paschen's raw giving a discharge start voltage is a function of the pd product.
  • FIG. 1 is a diagram for explaining a schematic configuration of an ozone generation apparatus according to an embodiment.
  • FIG. 2 is a diagram for explaining relations between the pd product and the ozone generation efficiency in the ozone generation apparatus according to the embodiment.
  • FIG. 3 is a diagram for explaining the relations between the pd product and the ozone generation efficiency in the ozone generation apparatus according to the embodiment in more detail.
  • An ozone generation apparatus includes a cylindrical shaped first electrode, a cylindrical shaped second electrode disposed coaxially with the first electrode and disposed in the first electrode, a dielectric disposed between the first electrode and the second electrode, and a power supply for applying a voltage between the first electrode and the second electrode. Dry air is supplied between the first electrode and the second electrode as raw material gas, a voltage is supplied between the first electrode and the second electrode from the power supply to generate discharge, and ozone is generated by the discharge.
  • a discharge gap length d formed by the first electrode, the second electrode, and the dielectric is set to be in a range of 0.3 to 0.5 mm.
  • a pd product which is a product of the discharge gap length d and a gas pressure p of the raw material gas, is in a range of 6 to 16 kPa ⁇ cm.
  • the discharge gap length d and the gas pressure p of the raw material gas are set to satisfy expression
  • FIG. 1 shows a schematic configuration of an ozone generation apparatus according to an embodiment.
  • An ozone generation apparatus 10 is an ozone generation apparatus of dielectric barrier discharge type. Roughly dividing, an ozone generation apparatus 10 includes an ozone generation apparatus main body 11 and a high voltage power supply 13 .
  • the high voltage power supply 13 is a high voltage AC power supply, and supplies power to the ozone generation apparatus main body 11 via a fuse 12 .
  • the ozone generation apparatus main body 11 includes an airtight vessel 15 .
  • a gas inlet 16 is provided in a first end portion of the airtight vessel 15 to introduce raw material gas.
  • a gas outlet 17 is provided in a second end portion of the airtight vessel 15 to eject unreacted raw material gas and ozone (O 3 ).
  • a cylindrical shaped metal electrode (first electrode) 23 made of stainless steel and a cylindrical shaped dielectric electrode 21 are disposed in the airtight vessel 15 . Both ends of the metal electrode 23 are hermetically joined to inside of the airtight vessel 15 . The metal electrode 23 and the airtight vessel 15 form an airtight region. The dielectric electrode 21 is disposed inside the metal electrode 23 . A predetermined discharge gap 22 is formed between an outer circumference face of the dielectric electrode 21 and the metal electrode 23 . By the way, a plurality of projections 23 A is formed on an inner circumference face of the metal electrode 23 to form and maintain the discharge gap 22 .
  • a cooling water inlet 24 which introduces cooling water and a cooling water outlet 25 which ejects cooling water are provided in a portion of the airtight vessel 15 opposed to an outer circumference face (rear face) of the metal electrode 23 .
  • the metal electrode 23 and the portion of the airtight vessel 15 opposed to the outer circumference face of the metal electrode 23 form a cooling water flow path 26 between the cooling water inlet 24 and the cooling water outlet 25 .
  • the dielectric electrode 21 includes a cylindrical shaped dielectric 21 A, a conductive electrode (second electrode) 21 B, and a high voltage feeding terminal 21 C.
  • the cylindrical shaped dielectric 21 A is formed of quartz glass or the like which is small in thermal expansion coefficient.
  • the conductive electrode 21 B is formed on an inner circumference face of the cylindrical shaped dielectric 21 A.
  • the conductive electrode 21 B is cylindrical shaped.
  • the high voltage feeding terminal 21 C is inserted into the cylindrical shaped dielectric 21 A, and connected to the conductive electrode 21 B. Furthermore, the high voltage feeding terminal 21 C is connected to the high voltage power supply 13 via the fuse 12 .
  • the cylindrical shaped dielectric 21 A is formed of quartz glass, borosilicate glass, high silica glass, aluminosilicate glass, ceramics or the like.
  • the conductive electrode 21 B is a conductive film formed on the inner circumference face of the cylindrical shaped dielectric 21 A by using a film forming method such as sputtering, thermal spraying, deposition, electroless plating, electroplating, or paintwork.
  • a film forming method such as sputtering, thermal spraying, deposition, electroless plating, electroplating, or paintwork.
  • gold, silver, copper, stainless steel, chrome, tin, zinc, nickel carbon, or aluminum is used as a conductive material.
  • the discharge gap length d corresponding to the distance of the discharge gap 22 is set equal to a value in the range of 0.3 to 0.5 mm which is shorter than a discharge gap length of a general conventional ozone generation apparatus in the range of 0.6 to 1 mm.
  • the raw material gas is gas that contains oxygen.
  • the raw material gas is dry air.
  • Raw material gas pressure p which is pressure of the raw material gas (air) is set to cause the pd product which is the product of the discharge gap length d and the raw material gas pressure p to be in the range of 6 to 16 kPa ⁇ cm.
  • the raw material gas pressure p (kpa) and the gap length d (cm) are set to satisfy the following expression.
  • FIG. 2 is a diagram for explaining relations between the pd product and the ozone generation efficiency in the ozone generation apparatus according to the embodiment.
  • the abscissa axis represents the pd product (kPa ⁇ cm) and the ordinate axis represents the ozone generation efficiency (g/kWh).
  • ozone generation is conducted by using the discharge gap length d as a parameter under the condition that the ozone concentration is 40 g/Nm 3 and the power density is 3 kW/m 2 and constant.
  • the ozone generation apparatus 10 of the present embodiment having a discharge gap length d shorter than a discharge gap length in the conventional ozone generation apparatus, if the discharge gap length d becomes shorter as indicated by 0.5 mm ⁇ 0.4 mm ⁇ 0.3 mm, the pd product shifts to a smaller value whereas the ozone generation efficiency increases.
  • the optimum value of the pd product falls to 7.6 kPa ⁇ cm.
  • the discharge gap length d is in the range of 0.3 to 0.5 mm
  • the pd product which is the product of the discharge gap length d and the gas pressure p of the raw material gas, is in the range of 6 to 16 kPa ⁇ cm.
  • the ozone generation efficiency ⁇ (g/kWh) must satisfy Expression (2) in a case where the discharge gap length d and the pd product are in the above-described ranges.
  • An ozone generation efficiency that is 10% lower than the highest ozone generation efficiency 75 g/kwh is 67 g/kWh. To obtain an ozone generation efficiency of at least 67 g/kWh, it is necessary according to Expression (2) to satisfy
  • the ozone generation apparatus can generate ozone with a high ozone generation efficiency of at least 67 g/kWh.
  • FIG. 3 is a diagram for explaining the relations between the pd product and the ozone generation efficiency ⁇ in the ozone generation apparatus according to the embodiment in more detail.
  • black circles ( ⁇ ) indicate experimental values and a solid line indicates a simulation result of an ozone generation simulator developed by the present inventors.
  • the discharge gap length d is in the range of 0.3 to 0.5 mm.
  • a conventionally used ring shaped spacer inserted into the discharge gap (space) cannot be used.
  • the spacer itself has a thickness in the range of 0.1 to 0.3 mm. If the spacer is provided on an outer circumference face of the dielectric electrode 21 , the spacer fills a gas passage space and consequently the raw material gas does not flow and ozone generation cannot be conducted.
  • At least three projections 23 A are formed on a circumference of the inner circumference face of the metal electrode 23 integrally with the metal electrode 23 as shown in FIG. 1 .
  • at least three projections are formed on a circumference of an outer circumference of the cylindrical shaped dielectric 21 A included in the dielectric electrode 21 integrally with the cylindrical shaped dielectric 21 A.
  • These projections have a height which is equal to the discharge gap length.
  • the above-described projection 23 A is formed by pressing a metal edge against a pipe made of stainless steel, which is the metal electrode 23 , and crushing the pipe. Furthermore, it is also possible to form the projection 23 A by using a dice having a cut in a part when manufacturing the metal electrode in extrusion of a pipe. In these cases, the projection 23 A is formed of the same material as the metal electrode 23 . The projection 23 A comes in contact with the outer circumference face of the cylindrical shaped dielectric 21 A.
  • the projection comes in contact with the inner circumference face of the metal electrode 23 .
  • the present embodiment it is possible to make the gas pressure p less than 0.3 MPa by using an area where the pd product is smaller than that in the conventional apparatus, even if a discharge gap length d in the range of 0.3 to 0.5 mm which is smaller than that in the conventional apparatus is used.
  • the thickness of the airtight vessel 15 (casing) in the ozone generation apparatus 10 can be made thin, and consequently it becomes possible to generate ozone with lightweight, inexpensiveness, and a high efficiency.
  • the conductive electrode 21 B in the dielectric electrode 21 is formed by means of a sputtering method using stainless steel as a target.
  • the dielectric electrode 21 which is the high voltage side electrode
  • a discharge power density W/S can be represented by Expression (6).
  • V* is a self-sustaining discharge voltage
  • V op is an applied voltage
  • C 0 is capacitance of the discharge gap per unit area
  • Cg is capacitance of glass per unit area.
  • the self-sustaining discharge voltage V* is represented by Expression (7).
  • V* 203 pd+ 900 ⁇ 400 exp( ⁇ pd/ 6.66) (7)
  • the self-sustaining discharge voltage V* becomes a function of the pd product.
  • the self-sustaining discharge voltage V* is proportionate to the pd product.
  • the discharge gap length d in the conventional ozone generation apparatus is 1.3 mm and 0.6 mm
  • the optimum value of the pd product for the ozone generation efficiency is 20 kPa ⁇ cm and nearly constant.
  • the discharge gap length d is made as small as 0.3 to 0.5 mm
  • the pd product which is the product of the discharge gap length d and the gas pressure p of the raw material gas, is made as small as 6 to 16 kPa
  • This pd product value is in the range of 0.3 to 0.8 times the conventional pd product value (20 kPa ⁇ cm). Therefore, the self-sustaining discharge voltage represented by Expression (7) becomes 0.3 times the conventional self-sustaining discharge voltage at minimum.
  • the discharge power density W/S which can be used according to Expression (6).
  • the apparatus volume is proportionate to the discharge power density W/S. In the case where the same cooling capacity as that of the conventional apparatus is used, therefore, it is necessary to use at least the same discharge power density W/S as that of the conventional apparatus.
  • the frequency of the power supply is set to 10 kHz or higher, the power supply generates a radio wave in general.
  • radio wave noise generated by the power supply can be suppressed and the ozone generation apparatus can generate ozone with a high efficiency by bringing the frequency of the power supply into the range of 1 to 3.5 kHz.
  • Ozone water by, for example, conducting bubbling of ozone gas O 3 generated in water.
  • Ozone formed by using the ozone generation apparatus 10 according to the embodiment, or ozone water utilizing the ozone is applied to, for example, water processing technology and the like and can be used to deodorize, decolor, and sterilize water to be processed.
  • the gas pressure p (kPa) of the raw material gas and the discharge gap length d (cm) satisfy the following expression. Therefore, the ozone generation apparatus can generate ozone with a high efficiency.
  • ozone can be generated with a stable ozone concentration and a high efficiency by forming the conductive electrode 21 B in the dielectric electrode 21 , which is the high voltage electrode, on the inner circumference face of cylindrical glass by means of the sputtering method using a conductor as a target.
  • the high voltage electrode formed on the inner face of the cylindrical shaped dielectric 21 A in the dielectric electrode 21 by means of a sputtering method using stainless steel as a target has excellent corrosion resistance. Thereby, it becomes possible to generate ozone with a stable ozone concentration and a high efficiency.
  • the conductive electrode 21 B may be a conductor formed on an inner circumference face of cylindrical glass, which is a dielectric, by plating.
  • the conductive electrode 21 B is nickel formed on the inner circumference face of cylindrical glass, which is a dielectric, by plating, the conductive electrode 21 B has excellent corrosion resistance and it becomes possible to generate ozone with a stable ozone concentration and a high efficiency.
  • the ozone generation apparatus can generate ozone with a high efficiency in a state in which radio wave noise generated by the high voltage power supply 13 is essentially suppressed, by setting the frequency of the high voltage power supply 13 in the range of 1 to 3.5 kHz.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Toxicology (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Oxygen, Ozone, And Oxides In General (AREA)
US14/487,445 2012-03-16 2014-09-16 Ozone generation apparatus Abandoned US20150004070A1 (en)

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JP2012059696A JP5677344B2 (ja) 2012-03-16 2012-03-16 オゾン発生装置
JP2012-059696 2012-03-16
PCT/JP2013/000805 WO2013136663A1 (ja) 2012-03-16 2013-02-14 オゾン発生装置

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CA (1) CA2867459A1 (ja)
IN (1) IN2014DN07683A (ja)
SG (1) SG11201405767TA (ja)
WO (1) WO2013136663A1 (ja)

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US9309118B2 (en) 2012-08-09 2016-04-12 Kabushiki Kaisha Toshiba Ozone generating apparatus
GB2534343A (en) * 2014-11-11 2016-07-27 Ozone Ind Ltd Ozone generator plate
EP3208233A1 (de) * 2016-02-17 2017-08-23 Xylem IP Management S.à.r.l. Ozonerzeugung bei hohen drücken
JP2017160097A (ja) * 2016-03-11 2017-09-14 株式会社東芝 オゾン発生装置
US9902616B2 (en) 2014-01-24 2018-02-27 Ngk Insulators, Ltd. Method for generating ozone

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JP2015137215A (ja) 2014-01-24 2015-07-30 日本碍子株式会社 オゾン発生器
JP6486843B2 (ja) * 2016-01-20 2019-03-20 株式会社東芝 オゾン発生装置および電源装置
EP3421417A1 (en) 2017-06-30 2019-01-02 SUEZ Groupe Method for controlling an ozone generating machine
EP3806586B1 (en) * 2018-05-30 2022-07-13 Toshiba Mitsubishi-Electric Industrial Systems Corporation Active gas generation device
JP6672447B2 (ja) * 2018-12-28 2020-03-25 株式会社東芝 オゾン発生装置および電源装置
CN114797406B (zh) * 2022-06-29 2022-09-13 浙大城市学院 一种自适应旋转电极低温等离子体反应器

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US9902616B2 (en) 2014-01-24 2018-02-27 Ngk Insulators, Ltd. Method for generating ozone
GB2534343A (en) * 2014-11-11 2016-07-27 Ozone Ind Ltd Ozone generator plate
EP3208233A1 (de) * 2016-02-17 2017-08-23 Xylem IP Management S.à.r.l. Ozonerzeugung bei hohen drücken
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SG11201405767TA (en) 2014-11-27
JP2013193893A (ja) 2013-09-30
WO2013136663A1 (ja) 2013-09-19
CA2867459A1 (en) 2013-09-19
JP5677344B2 (ja) 2015-02-25
US20160236933A1 (en) 2016-08-18
US10759661B2 (en) 2020-09-01

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