WO2015012106A1 - 水電解用の多孔質導電部材、及び、それを用いた機能水生成器 - Google Patents

水電解用の多孔質導電部材、及び、それを用いた機能水生成器 Download PDF

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Publication number
WO2015012106A1
WO2015012106A1 PCT/JP2014/068290 JP2014068290W WO2015012106A1 WO 2015012106 A1 WO2015012106 A1 WO 2015012106A1 JP 2014068290 W JP2014068290 W JP 2014068290W WO 2015012106 A1 WO2015012106 A1 WO 2015012106A1
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WIPO (PCT)
Prior art keywords
porous
water electrolysis
conductive member
water
binder material
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Application number
PCT/JP2014/068290
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English (en)
French (fr)
Japanese (ja)
Inventor
加藤　康昭
寺島　健太郎
矢野　裕嗣
勇人 砂子
翔子 橋爪
輝男 内堀
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シャープ株式会社
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Application filed by シャープ株式会社 filed Critical シャープ株式会社
Priority to CN201480041197.1A priority Critical patent/CN105392926A/zh
Publication of WO2015012106A1 publication Critical patent/WO2015012106A1/ja

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    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/4618—Devices therefor; Their operating or servicing for producing "ionised" acidic or basic water
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
    • C25B11/03—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form perforated or foraminous
    • C25B11/031—Porous electrodes
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/005—Systems or processes based on supernatural or anthroposophic principles, cosmic or terrestrial radiation, geomancy or rhabdomancy
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46152—Electrodes characterised by the shape or form
    • C02F2001/46157—Perforated or foraminous electrodes
    • C02F2001/46161—Porous electrodes

Definitions

  • the present invention is for water electrolysis comprising a porous conductor portion including a hydrophilized electrode active material and a binder material, and a current collector portion in contact with or included in the surface of the porous conductor portion.
  • a porous electroconductive member for water electrolysis wherein the binder material is composed of a hydrophobic material, and a one-tank membrane type using the electroconductive member for water electrolysis It is related with the functional water generator which produces
  • an electrode material of an electric double layer capacitor it has been common to use activated carbon or the like as an electrode active material and to perform molding using a fluorine-based hydrophobic binder material.
  • activated carbon or the like As an electrode material of an electric double layer capacitor, it has been common to use activated carbon or the like as an electrode active material and to perform molding using a fluorine-based hydrophobic binder material.
  • the binder material In electrolysis using tap water or the like as raw water, when a fluororesin binder material such as polytetrafluoroethylene is used as the hydrophobic binder material, the binder material has water repellency. There was a problem that the impregnation property was poor and predetermined electrical characteristics could not be obtained in electrolysis or the like.
  • both the binder material and the activated carbon are hydrophilic, so the affinity between the binder material and the activated carbon is increased. For this reason, if the content of the hydrophilic binder material in the electrode is increased so that the activated carbon is not lost, it becomes easier for the hydrophilic binder material to cover the activated carbon surface, reducing the effective ion adsorption pores of the activated carbon and greatly reducing the adsorption performance.
  • the electrolytic efficiency cannot be maximized.
  • the present invention has been made in order to solve the above-mentioned problems, and the object of the present invention is to improve the electrolysis efficiency while using a hydrophobic binder material which has been conventionally considered unsuitable for water electrolysis. It is to provide a porous conductive member for water electrolysis.
  • the porous electroconductive member for water electrolysis includes a porous conductor portion containing a hydrophilized electrode active material and a binder material, and a collection in contact with or included in the surface of the porous conductor portion.
  • a porous electroconductive member for water electrolysis comprising an electric body portion, wherein the binder material is made of a hydrophobic material.
  • the electrode active material is contained in the porous conductor portion at 70 wt% or more and 92 wt% or less.
  • the binder material is preferably a fluorine-based material.
  • the porous conductor portion further contains 5 wt% or more of a conductive additive.
  • the porous conductor portion preferably has a thickness of a thickest portion of 0.5 mm or more and 1.5 mm or less.
  • the thickness of the thickest portion of the porous conductor portion is approximately 1.0 mm.
  • porous conductive member for water electrolysis it is preferable to provide a plurality of the current collector portions with respect to the porous conductor portion.
  • the current collector portion is preferably a metal member without a noble metal coat.
  • the porous electroconductive member for water electrolysis according to the present invention is preferably manufactured by performing a surface treatment after roll rolling to make it hydrophilic.
  • the present invention also provides a functional water generator provided with the above-described porous electroconductive member for water electrolysis according to the present invention as an electrode for adsorbing and desorbing metal ions in a single-cell membrane electrolytic cell.
  • the functional water generator of the present invention is preferably used for dishwashing, hairdressing, moisturizing or drinking.
  • the porous conductor part including the electrode active material and the binder material subjected to the hydrophilic treatment, and the surface of the porous conductor part are provided.
  • a porous electroconductive member for water electrolysis comprising an abutting or enclosing current collector portion, wherein the binder material is made of a hydrophobic material, so that the adsorption performance of the electrode active material can be maximized .
  • the thickness of the thickest portion of the porous conductor portion is 0.5 mm or more and 1.5 mm or less.
  • the present invention also provides a functional water generator that generates functional water for use in dishwashing, hairdressing, humidification, or drinking, to which the conductive member for water electrolysis of the present invention is suitably applied. can do.
  • FIG. 1 (a) is a diagram schematically showing a porous electroconductive member 1 for water electrolysis as a preferred example of the present invention
  • FIG. 1 (b) is an enlarged view of a part of FIG. 1 (a).
  • FIG. 1 (a) is a diagram schematically showing a porous electroconductive member 1 for water electrolysis as a preferred example of the present invention
  • FIG. 1 (b) is an enlarged view of a part of FIG. 1 (a). It is a photograph (3000 times magnified photograph by a scanning electron microscope).
  • the porous electroconductive member 1 for water electrolysis according to the present invention is in contact with a porous conductor portion 2 including a hydrophilized electrode active material 4 and a binder material 5, and the surface of the porous conductor portion 2.
  • the current collector section 3 is included (the embodiment shown in FIG. 1A is referred to as “embodiment 1”).
  • FIG. 2 is a graph showing the result of actually comparing the ion adsorption characteristics between the porous conductor portion using the hydrophilic binder material and the porous conductor portion using the hydrophobic binder material.
  • the vertical axis represents ion treatment efficiency (%), and the horizontal axis represents ion treatment time (minutes).
  • the ion treatment efficiency here means the ion desorption efficiency when desorption is performed after performing ion adsorption at a predetermined level or more in the porous conductor portion.
  • FIG. 3 is a photograph (3000 times magnified photograph taken with a scanning electron microscope) showing the porous conductor portion when a hydrophobic binder material and a hydrophilic electrode active material are used.
  • the binder material since the hydrophilic electrode active material and the hydrophobic binder material have low affinity, the binder material does not include the electrode active material and the electrode active material is easily exposed. It is easy to maintain the pore structure of the substance and the gap between the electrode active materials. Therefore, it is possible to suppress the reduction of effective ion adsorption holes and maximize the electrolysis efficiency.
  • any electrode active material conventionally used in the art can be used without particular limitation, but particulate activated carbon is preferable.
  • Activated carbon plays an important role in improving the energy density of the electrode, and the type thereof is not particularly limited, and phenolic, rayon-based, acrylic-based, pitch-based, coconut shell-based, etc. can be used, and the specific surface area is preferably 300-3500 m 2 / g, more preferably 1500-2500 m 2 / g can be used.
  • the specific surface area of the electrode active material is less than 300 m 2 / g, the ion adsorption performance tends to deteriorate.
  • the specific surface area of the electrode active material exceeds 3500 m 2 / g, it is considered that the ion adsorption performance is reduced, and the ratio of the electrode active material to the porous conductor portion increases, so that the porous conductor portion There is a tendency for the formability of the resin to be lowered and the workability to be lowered. Particularly when the specific surface area of the electrode active material is 1500 to 2500 m 2 / g, the ion adsorption performance can be preferably improved.
  • the average particle diameter of the electrode active material 4 in the present invention is not particularly limited, but it is within the range of 1 to 45 ⁇ m because it is easy to form a thin film and the capacity density can be increased. Preferably, it is in the range of 2 to 40 ⁇ m, more preferably in the range of 3 to 20 ⁇ m.
  • the electrode active material 4 in the present invention is subjected to a hydrophilization treatment, and this hydrophilization treatment is performed by a method such as high-temperature activation of sodium hydroxide or water vapor, for example.
  • the electrode active material 4 is improved in wettability with respect to water by the hydrophilic treatment by activation, and can effectively perform ion adsorption on the surface of the electrode active material made porous by activation.
  • the current collector 3 may be in contact with the porous conductor 2 or may be encapsulated (inserted / inserted). In the case of contact, in order to prevent electrolysis from occurring in the current collector, it is desirable to insulate by attaching a polyimide tape or the like.
  • the hydrophobic material constituting the binder material 5 is preferably a fluorine-based material.
  • the fluorine-based material include polytetrafluoroethylene (PTFE), and the fluorine-based material is hydrophobic and is made into a fiber (fibrillation) by applying a shear (shearing force) during heat molding. Therefore, networkability can improve the moldability of the porous conductor portion and suppress the elution of the electrode active material from the porous conductor portion.
  • tetrafluoroethylene When PTFE is used as the hydrophobic material constituting the binder material 5, not only a tetrafluoroethylene homopolymer but also 0.5 mol% or less of other monomers are added to tetrafluoroethylene for copolymerization. It may be a copolymer. Examples of these other monomers include trifluoroethylene, (perfluoroalkyl) ethylene, chlorotrifluoroethylene, hexafluoropropylene, and perfluoro (alkyl vinyl ether).
  • the electrode active material 4 is preferably contained in the porous conductor portion 2 in an amount of 70 wt% or more and 92 wt% or less, and is contained in an amount of 80 wt% or more and 92 wt% or less. It is more preferable.
  • FIG. 4 is a graph showing the relationship between the content rate and ion treatment efficiency when activated carbon is used as the electrode active material, the vertical axis represents the ion treatment efficiency (%), and the horizontal axis represents the activated carbon content. The rate (wt%) is shown. As shown in FIG. 4, by setting the content ratio of the electrode active material (activated carbon in the example of FIG.
  • the content ratio of the electrode active material in the porous conductor portion is 70 wt%, the binder
  • the content of the material is 27 wt% (conducting aid: 3 wt%)
  • the ion treatment efficiency is about 80%.
  • the electrode active material 4 is removed from the porous conductor portion 2. It is possible to substantially suppress the elution, and in this case, it is possible to maintain almost 100% as the ion processing efficiency.
  • the binder material 5 by forming the binder material 5 with a hydrophobic material such as PTFE, the blending ratio of the binder material 5 can be reduced as much as possible, and the content ratio of the electrode active material can be increased as high as 70 wt% or more and 92 wt% or less. Therefore, it is preferable from the viewpoint of ion processing efficiency.
  • a hydrophobic material such as PTFE
  • the porous conductor portion 2 further contains 5 wt% or more of a conductive additive.
  • a conductive additive improves electron transfer between adjacent electrode active materials, which is preferable from the viewpoint of ion treatment efficiency.
  • a material having high electrical conductivity such as carbon black can be used. Since carbon black imparts conductivity to the electrode and contributes to a reduction in internal resistance, it is sufficient that the carbon black has excellent conductivity, such as acetylene black or ketjen black. A thickness of 01 to 1 ⁇ m is preferable.
  • FIG. 5 is a graph showing the relationship between the content of the conductive assistant and the ion treatment efficiency when activated carbon is fixed as the electrode active material 4 at a content of 70 wt% and carbon black is used as the conductive assistant.
  • the vertical axis represents ion treatment efficiency (%), and the horizontal axis represents the content (wt%) of the conductive additive.
  • the ion treatment efficiency is almost constant until the content of the conductive auxiliary is 5 wt%, but increases from the content of the conductive auxiliary of 5 wt%, and the ion treatment efficiency is increased when the content of the conductive auxiliary is 10 wt%. Increases by more than 10%.
  • the content of the conductive assistant is preferably 5 wt% or more, and more preferably 10 wt% or more.
  • the porous electroconductive member 1 for water electrolysis of the present invention has a porous conductor part from the viewpoint of solving the problem that water does not permeate into the adsorption electrode, which is a problem when a hydrophobic binder material is used.
  • the thickness of the thickest part 2 is preferably 0.5 mm or more and 1.5 mm or less.
  • “the thickness of the thickest portion” of the porous conductor portion 2 is a porous conductor in a direction (thickness direction) perpendicular to a plane parallel to the current collector portion 3 of the porous conductor portion 2. The straight line distance between the end of the part 2 and the current collector part 3 is indicated.
  • FIG. 6 is a graph showing the relationship between the thickness of the thickest portion of the porous conductor portion and the ion treatment efficiency when the electrolysis time is 4 minutes, 6 minutes, and 8 minutes, and the vertical axis represents the ion treatment efficiency. (%), The horizontal axis indicates the thickness (mm) of the thickest portion of the porous conductor portion.
  • the ion treatment efficiency is high in any electrolysis time within the range where the thickness of the thickest part of the porous conductor portion is 0.5 mm or more and 1.5 mm or less, but outside this range, Ion processing efficiency becomes worse.
  • the porous electroconductive member 1 for water electrolysis according to the present invention is preferably ion-treated by setting the thickest portion of the porous conductor portion to 0.5 mm or more and 1.5 mm or less. Efficiency can be improved.
  • Q is the amount of electricity (C)
  • I is the amount of current (A)
  • t is the time (sec)
  • n is the molar amount of the metal ion
  • the porous electroconductive member for water electrolysis of the present invention has the maximum ion treatment efficiency by setting the thickness of the thickest part to approximately 1.0 mm, that is, within the range of 0.8 mm to 1.2 mm. It is possible to
  • FIG. 7 is a diagram schematically showing porous electroconductive members 1, 11, 21, 31 for water electrolysis of various preferable examples of the present invention.
  • FIG. 7A shows an embodiment 1 similar to that shown in FIG. 1A (porous electroconductive member 1 for water electrolysis), and FIG. 7B shows an embodiment. 2 (porous electroconductive member 11 for water electrolysis),
  • FIG. 7 (c) shows Embodiment 3 (porous electroconductive member 21 for water electrolysis), and
  • FIG. 7 (d) shows Embodiment 4 ( A porous conductive member 31) for water electrolysis is shown.
  • FIG. 7 shows the thickness direction of the porous conductive member (the direction perpendicular to the plane parallel to the current collector portion 3) in the vertical direction with respect to the paper surface.
  • FIG. 7A shows a case where the current collector portion 3 is brought into contact with the surface of the porous conductor portion 2, and FIG. 7B shows the inside of the porous conductor portion 12.
  • FIGS. 7 (c) and 7 (d) show a configuration in which a plurality of current collector portions are provided as in the examples shown in FIGS. 7 (c) and 7 (d).
  • FIG. 7 (c) the two current collector parts 23, 24 are placed inside the porous conductor part 22 so as to be spaced apart (2d in FIG. 7 (c)).
  • FIG. 7 (d) shows three current collectors that are spaced from each other (2d in FIG.
  • the distance d is synonymous with the above-mentioned “thickness of the thickest portion”, and is preferably in the range of 0.5 mm or more and 1.5 mm or less.
  • the distance between the current collectors is 2d (that is, the thickness of the thickest portion). 2 times) is preferable.
  • the current collector does not necessarily need a noble metal coat such as a platinum coat.
  • the current collector portion may be a metal member without a noble metal coat, and a metal such as stainless steel or titanium metal that is easily eluted by the electrolytic solution is used as it is. Therefore, the electrode cost can be reduced.
  • the porous electroconductive member for water electrolysis according to the present invention is preferably manufactured by subjecting it to surface treatment after roll rolling to make it hydrophilic.
  • the porous electroconductive member for water electrolysis of the present invention is obtained by rolling a precursor of a porous electroconductive portion containing an electrode active material and a hydrophobic binder material, and obtaining the sheet-like material (porous electroconductive sheet) Moreover, it can manufacture suitably by performing a hydrophilic treatment as surface treatment.
  • the hydrophilic treatment method for the porous conductive sheet include metal sodium solution treatment, EB irradiation treatment, plasma treatment, excimer laser treatment, ultraviolet laser treatment, corona treatment, and sulfonation treatment.
  • the inside of an electrode can be adsorbed by hydrophilizing the porous conductive sheet to obtain the porous electroconductive member for water electrolysis of the present invention.
  • FIG. 8 is a diagram schematically showing a functional water generator 51 of a preferred example using the porous electroconductive member for water electrolysis of the present invention.
  • the present invention also provides a functional water generator provided with the above-described porous electroconductive member for water electrolysis according to the present invention as an electrode for adsorbing and desorbing metal ions in an electrolyzer having a single diaphragm.
  • the functional water generator 51 of the example shown in FIG. 8 includes an electrolyzer 52 of a non-diaphragm 1 tank type including the porous conductive members 1, 11, 21, 31 of the present invention described above and a platinum electrode 54.
  • the 8 is a constant current generator for supplying a current that is electrically connected to the porous conductive members 1, 11, 21, 31 and the platinum electrode 54 in the electrolytic cell 52.
  • the control device 57 is provided.
  • the constant current generation source 55, the switching circuit 56, and the control device 57 may be used in combination with appropriate ones known in the art, and are not particularly limited.
  • the platinum electrode is used as the anode / cathode and the porous conductive member for water electrolysis is used as the cathode / cathode with respect to the raw water (for example, tap water) supplied into the electrolytic vessel.
  • Acidic / alkaline water can be generated by electrolysis using the anode.
  • “Functional water” as used in the present invention is a generic term for this acidic water and alkaline water.
  • the electrode tank can be simplified, and in principle, no waste water is generated. It is possible to produce water such as acidic / alkaline water.
  • the functional water generator of the present invention is characterized in that it is used for dishwashing, hairdressing, humidification, or drinking.
  • the porous electroconductive member for water electrolysis according to the present invention the moldability of the binder material is strong, and it is possible to substantially suppress the elution of the electrode active material from the porous conductor portion. Therefore, there is little problem of elution even in applications where contamination with impurities such as dishwashing use, barber / beauty use, humidification use, or drinking use is a problem.
  • Porous conductive member for water electrolysis 1, 11, 21, 31, 53 Porous conductive member for water electrolysis, 2, 12, 22, 32 Porous conductor part, 3, 13, 23, 33 Current collector part 4, Electrode active material, 5 Binder Material, 51 functional water generator, 52 electrolyzer, 54 platinum electrode, 55 constant current source, 56 switching circuit, 57 control circuit.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Hydrology & Water Resources (AREA)
  • Environmental & Geological Engineering (AREA)
  • Water Supply & Treatment (AREA)
  • Water Treatment By Electricity Or Magnetism (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
PCT/JP2014/068290 2013-07-26 2014-07-09 水電解用の多孔質導電部材、及び、それを用いた機能水生成器 WO2015012106A1 (ja)

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JP2013155728A JP2015025174A (ja) 2013-07-26 2013-07-26 水電解用の多孔質導電部材、及び、それを用いた機能水生成器
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RU2647841C2 (ru) * 2016-08-11 2018-03-21 Публичное акционерное общество "Ракетно-космическая корпорация "Энергия" имени С.П. Королёва (ПАО "РКК "Энергия") Электролизёр воды и способ его эксплуатации
CN109631651B (zh) * 2018-12-06 2020-07-07 华北电力大学 一种局部自适应可控浸润性耦合微结构强化沸腾换热方法
JP2021070863A (ja) * 2019-11-01 2021-05-06 東洋アルミニウム株式会社 アルカリ水電解用電極

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JP2006051457A (ja) * 2004-08-13 2006-02-23 Fuji Photo Film Co Ltd 銀担持触媒及びその製造方法並びに銀触媒担持型ガス拡散電極及びそれを用いた電解酸化処理方法と電解酸化装置
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Publication number Priority date Publication date Assignee Title
JPS6075593A (ja) * 1983-06-22 1985-04-27 アトケム 導電性繊維を主体とする陰極要素の製造方法
JP2005505692A (ja) * 2001-10-02 2005-02-24 バイエル マテエリアルサイエンス アーゲー ガス拡散電極の製造方法
JP2006051457A (ja) * 2004-08-13 2006-02-23 Fuji Photo Film Co Ltd 銀担持触媒及びその製造方法並びに銀触媒担持型ガス拡散電極及びそれを用いた電解酸化処理方法と電解酸化装置
JP2006219694A (ja) * 2005-02-08 2006-08-24 Permelec Electrode Ltd ガス拡散電極
WO2011013578A1 (ja) * 2009-07-31 2011-02-03 旭硝子株式会社 電解質材料、液状組成物および固体高分子形燃料電池用膜電極接合体
JP2013108104A (ja) * 2011-11-17 2013-06-06 Permelec Electrode Ltd 電解合成装置、電解処理装置、電解合成方法及び電解処理方法

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