US20220178034A1 - Electrode for electrolysis, and method for producing electrode for electrolysis - Google Patents

Electrode for electrolysis, and method for producing electrode for electrolysis Download PDF

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US20220178034A1
US20220178034A1 US17/604,426 US202017604426A US2022178034A1 US 20220178034 A1 US20220178034 A1 US 20220178034A1 US 202017604426 A US202017604426 A US 202017604426A US 2022178034 A1 US2022178034 A1 US 2022178034A1
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layer
tantalum
layers
electrically conductive
conductive substrate
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Mohd ERMAN
Fumitoshi SHINNO
Hiroshi Adachi
Yoshiharu Sanagawa
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Panasonic Intellectual Property Management Co Ltd
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Panasonic Intellectual Property Management Co Ltd
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    • 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
    • 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
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/055—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material
    • C25B11/057—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material consisting of a single element or compound
    • C25B11/061—Metal or alloy
    • C25B11/063—Valve metal, e.g. titanium
    • 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
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C25B1/01—Products
    • C25B1/24—Halogens or compounds thereof
    • C25B1/26—Chlorine; Compounds thereof
    • 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
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/052—Electrodes comprising one or more electrocatalytic coatings on a substrate
    • C25B11/053—Electrodes comprising one or more electrocatalytic coatings on a substrate characterised by multilayer electrocatalytic coatings
    • 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
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/055—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material
    • C25B11/069—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material consisting of at least one single element and at least one compound; consisting of two or more compounds
    • 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
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
    • C25B11/075—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of a single catalytic element or catalytic compound
    • C25B11/081—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of a single catalytic element or catalytic compound the element being a noble metal
    • 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
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
    • C25B11/091—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
    • C25B11/093—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds at least one noble metal or noble metal oxide and at least one non-noble metal oxide

Definitions

  • the electrode for electrolysis is desired to be less likely to cause the separation of the composite layer, which contains Iridium serving as a catalyst, in order to increase the life-time of the electrode.
  • FIG. 8 is a sectional view of an electrode for electrolysis according to a variation.
  • the composite layer 4 has a bottom layer closest to the primary surface 21 of the electrically conductive substrate 2 .
  • the bottom layer of the composite layer 4 is constituted by one tantalum layer 41 of the plurality of tantalum layers 41 .
  • the composite layer 4 has a top layer furthest from the electrically conductive substrate 2 .
  • the top layer of the composite layer 4 is constituted by one catalyst layer 42 of the plurality of catalyst layers 42 .
  • one tantalum layer 41 (first tantalum layer 411 ) of the plurality of tantalum layers 41 constitutes the bottom layer that is closest to the first primary surface 21 of the electrically conductive substrate 2 .
  • one catalyst layer 42 (fourth catalyst layer 424 , in the illustrated example) of the plurality of catalyst layers 42 constitutes the top layer that is furthest from the electrically conductive substrate 2 .
  • the compound layer formation process includes forming the composite layer 4 on the intermediate layer 3 (see FIG. 3D ).
  • the compound layer formation process includes a stacked body formation process and a firing process.
  • the stacked body formation process includes performing a first prescribed number of times (four times, for example) of first steps and a second prescribed number of times (four times, for example) of second steps, where the first step and the second step are performed alternately, to form, on the intermediate layer 3 which is on the electrically conductive substrate 2 , a stacked body 400 (see FIG. 3C ) serving as a basis of the composite layer 4 .
  • the first step includes applying a solution (hereinafter, referred to as “first solution”) containing a tantalum compound serving as a basis of the tantalum layer 41 , and subsequently performing, without natural drying, heat treatment (drying process) of heating and drying under a first condition, to form a first material layer 410 serving as a basis of one tantalum layer 41 of the plurality of tantalum layers 41 .
  • the first solution is a solution obtained by dissolving the tantalum compound in a solvent (hereinafter, referred to as “first solvent”).
  • the first solvent is a liquid of a mixture of ethylene glycol monoethyl ether, hydrochloric acid and ethanol, for example.
  • the tantalum compound is for example tantalum chlorine, but is not limited thereto.
  • the tantalum compound may be tantalum ethoxydo, for example.
  • the metal concentration (tantalum concentration) of the first solution is 26 mg/L, for example.
  • the application amount of the first solution is 1 ⁇ L/cm 2 , for example.
  • the first condition includes a heat treatment temperature and a heat treatment time.
  • the heat treatment temperature of the first condition falls within a range of 100° C. to 400° C. for example, and the heat treatment temperature may be 220° C. as an example.
  • the heat treatment time of the first condition falls within a range of 5 minutes to 15 minutes for example, and the heat treatment time may be 10 minutes as an example.
  • the second step includes applying a solution (hereinafter, referred to as “second solution”) containing a platinum compound and iridium compound serving as a basis of the catalyst layer 42 , and subsequently performing, without natural drying, heat treatment (drying process) of heating and drying under a second condition, to form a second material layer 420 serving as a basis of one catalyst layer 42 of the plurality of catalyst layers 42 .
  • the second solution is a solution obtained by dissolving the platinum compound and the iridium compound in a solvent (hereinafter, referred to as “second solvent”).
  • the second solvent is a liquid of a mixture of ethylene glycol monoethyl ether, hydrochloric acid and ethanol, for example.
  • the platinum compound is for example hydrogen chloroplatinate, but is not limited thereto.
  • the platinum compound may be platinum chloride, for example.
  • the iridium compound is for example hydrogen chloroidiate, but is not limited thereto.
  • the iridium compound may be iridium chloride, iridium nitrate, or the like, for example.
  • the metal concentration (total of platinum concentration and iridium concentration) of the second solution is 26 mg/L, for example.
  • the application amount of the second solution is 2 ⁇ L/cm 2 , for example.
  • the second condition includes a heat treatment temperature and a heat treatment time.
  • the heat treatment temperature of the second condition falls within a range of 100° C. to 400° C. for example, and the heat treatment temperature may be 220° C. as an example.
  • the heat treatment time of the second condition falls within a range of 5 minutes to 15 minutes for example, and the heat treatment time may be 10 minutes as an example.
  • the firing process includes performing thermal treatment of firing the stacked body 400 under a predetermined firing condition to form the composite layer 4 and a plurality of cracks (recesses 5 ) (see FIG. 3D ).
  • the firing condition includes a firing temperature and a firing time.
  • the firing temperature falls within a range of 500° C. to 700° C. for example, and the firing temperature may be 560° C. as an example.
  • the firing time falls within a range of 10 minutes to 20 minutes for example, and the firing time may be 15 minutes as an example.
  • the plurality of cracks (recesses 5 ) may have mutually different shapes.
  • the crack may be formed along a thickness direction of the composite layer 4 or may be at least partially curved in the composite layer 4 .
  • Example 2 relates to a sample whose molar ratio of Pt:Ir:Ta is 8:1:6 and the number of layers is 20;
  • Example 3 relates to a sample whose molar ratio of Pt:Ir:Ta is 8:1:6 and the number of layers is 30;
  • Example 4 relates to a sample whose molar ratio of Pt:Ir:Ta is 8:3:6 and the number of layers is 10;
  • Example 5 relates to a sample whose molar ratio of Pt:Ir:Ta is 8:3:6 and the number of layers is 20;
  • Example 6 relates to a sample whose molar ratio of Pt:Ir:Ta is 8:3:6 and the number of layers is 30;
  • Example 7 relates to a sample whose molar ratio of Pt:Ir:Ta is 8:5:6 and the number of layers is 10;
  • Example 8 relates to a sample whose molar ratio of Pt:Ir:Ta is 8:5:6 and the number of layers is 20;
  • Example 9 relates to a sample whose molar ratio of Pt:Ir:Ta is 8:5:6 and the number of layers is 30.
  • the durability test was conducted according to the accelerated test.
  • two electrodes for electrolysis 1 were produced in a same condition and used as a pair of electrodes. Firstly, the pair of electrodes were immersed in salt water inside a tank for electrolytic cell for a durability test apparatus, and an electric current was supplied between the pair of electrodes to conduct an initial aging.
  • the electric current was supplied between the pair of electrodes for total twelve minutes, where the polarity was reversed every time a predetermined time (3 minutes) elapses.
  • the feature “the polarity is reversed” used herein indicates that the roles of the pair of electrodes, the anode or the cathode, are mutually interchanged.
  • the feature “the polarity is reversed” indicates that an electrode (to be) used as the higher potential side electrode is changed from one of the pair of electrodes to the other thereof, such that one of the electrodes which has been used as the anode is to be used as the cathode, and vice verse.
  • the horizontal axis of FIG. 4 indicates the durability test time (elapsed time) after the initial aging.
  • the vertical axis of FIG. 4 indicates the chlorine concentration. It should be noted that the chlorine generated around the anode is to be used for the generation of hypochlorous acid. Thus, the chlorine concentration substantially reflects the amount of chlorine, which has been produced during a recent unit time.
  • FIGS. 5A, 5B, 5C and 5D Based on FIGS. 5A, 5B, 5C and 5D , an inferred mechanism is described which can explain a reason why the electrode for electrolysis 1 according to the first embodiment has an improved durability.
  • FIGS. 5A, 5B, 5C, and 5D are ordered according to the time series.
  • respective sides of a plurality of (four) catalyst layers 42 that partially form an inner surface of the recess 5 , as well as the main surface 40 , of the composite layer 4 are in contact with the salt water.
  • Each of the plurality of (four) catalyst layers 42 thus can contribute to the generation of the chlorine.
  • FIG. 5B shows a state of the electrode for electrolysis 1 where a catalyst layer 42 (fourth catalyst layer 424 ) of the top layer shown in FIG. 5A is lost.
  • a catalyst layer 42 fourth catalyst layer 424
  • respective sides of a plurality of (three) catalyst layers 42 that partially form an inner surface of the recess 5 are in contact with the salt water.
  • Each of the plurality of (three) catalyst layers 42 thus can contribute to the generation of the chlorine.
  • FIG. 5C shows a state where the plurality of (three) catalyst layers 42 are partially lost in an in-plane direction, from the state shown in FIG. 5B .
  • the in-plane direction is defined as a direction perpendicular to the thickness direction D 1 of the electrically conductive substrate 2 . That is, the in-plane direction is a direction along the first primary surface 21 of the electrically conductive substrate 2 .
  • respective sides, closer to the recess 5 of the plurality of (three) catalyst layers 42 are in contact with the salt water.
  • Each of the plurality of (three) catalyst layers 42 thus can contribute to the generation of the chlorine.
  • FIG. 5D shows a state where a tantalum layer 41 (fourth tantalum layer 414 ) on a catalyst layer 42 (third catalyst layer 423 ), which is furthest from the electrically conductive substrate 2 , of the plurality of (three) catalyst layers 42 is partially lost along the in-plane direction, from the state shown in FIG. 5C .
  • respective sides, closer to the recess 5 , of the plurality of (three) catalyst layers 42 , as well as a main surface of the third catalyst layer 423 closer to the fourth tantalum layer 414 are in contact with the salt water.
  • Each of the plurality of (three) catalyst layers 42 thus can contribute to the generation of the chlorine.
  • At least one of the catalyst layers 42 always can contribute to the generation of the chlorine, regardless of the change in the state thereof.
  • the electrode for electrolysis 1 according to the first embodiment thus can have an improved durability.
  • the electrode for electrolysis 1 according to the first embodiment includes the composite layer 4 alternating the plurality of tantalum layers 41 and the plurality of catalyst layers 42 one layer by one layer, which can contribute to suppress the separation of the composite layer 4 .
  • the electrode for electrolysis 1 according to the first embodiment includes the composite layer 4 , which also can contribute to suppress the waste of the composite layer 4 in use.
  • the electrode for electrolysis 1 according to the first embodiment includes the composite layer 4 , which also can contribute to suppress the cohesion of iridium.
  • the electrode for electrolysis 1 according to the first embodiment has the plurality of recesses 5 , which can increase the area of the surface of the composite layer 4 contributing the generation of the chlorine, and can contribute to improve the chlorine generation efficiency.
  • the electrode for electrolysis 1 a according to the second embodiment is substantially the same as the electrode for electrolysis 1 according to the first embodiment.
  • the electrode for electrolysis 1 a according to the second embodiment differ from the electrode for electrolysis 1 according to the first embodiment in the depths of the recesses 5 .
  • Components of the electrode for electrolysis 1 a according to the second embodiment similar to those of the electrode for electrolysis 1 according to the first embodiment are assigned same reference signs and explanation thereof may be omitted.
  • Each of the plurality of recesses 5 of the electrode for electrolysis 1 a according to the second embodiment has a depth which is smaller than or equal to a distance L 3 between a main surface 40 of a composite layer 4 and a bottom layer (first tantalum layer 411 ) of the composite layer 4 . This can contribute to further suppression of the separation of the composite layer 4 according to the electrode for electrolysis 1 a according to the second embodiment.
  • a method for producing the electrode for electrolysis 1 a according to the second embodiment is explained with reference to FIGS. 7A to 7E . It may be omitted the detailed explanation of some of processes, similar to those of the method for producing the electrode for electrolysis 1 according to the first embodiment.
  • An electrically conductive substrate 2 is prepared firstly as shown in FIG. 7A , and a roughening process, an intermediate layer formation process, and a composite layer formation process are performed sequentially after the preparation.
  • the compound layer formation process includes a first process, a second process, and a third process.
  • the tantalum compound may be tantalum ethoxydo, for example.
  • the solution may be obtained by dissolving pure tantalum in the solvent, for example, which can form the tantalum layer 41 as a layer made from tantalum, instead of a layer made from tantalum oxide.
  • the metal concentration (tantalum concentration) of the solution is 26 mg/L, for example.
  • the application amount of the solution is 1 ⁇ L/cm 2 , for example.
  • the firing condition includes a firing temperature (first prescribed temperature) and a firing time.
  • the firing temperature falls within a range of 500° C. to 700° C. for example, and the firing temperature may be 560° C. as an example.
  • the firing time falls within a range of 10 minutes to 20 minutes for example, and the firing time may be 15 minutes as an example.
  • the first step of the second process includes applying a second solution containing a platinum compound and iridium compound serving as a basis of a catalyst layer 42 , and subsequently performing, without natural drying, heat treatment (drying process) of heating and drying under a second condition to form a second material layer 420 serving as a basis of one catalyst layer 42 of the plurality of catalyst layers 42 .
  • the second solution contains platinum and iridium.
  • the second solution is applied to a layer (a tantalum layer 41 as a bottom layer, or a first material layer 410 described later, for example) exposed outside on a side of the first primary surface 21 of the electrically conductive substrate 2 .
  • the second condition includes a heat treatment temperature and a heat treatment time.
  • the heat treatment temperature (second prescribed temperature) of the second condition falls within a range of 100° C. to 400° C. for example, and the heat treatment temperature may be 220° C. as an example.
  • the heat treatment time of the second condition falls within a range of 5 minutes to 15 minutes for example, and the heat treatment time may be 10 minutes as an example.
  • the second step of the second process includes applying a first solution containing a tantalum compound serving as a basis of the tantalum layer 41 , and subsequently performing, without natural drying, heat treatment (drying process) of heating and drying under a first condition, to form a first material layer 410 serving as a basis of one tantalum layer 41 of the plurality of tantalum layers 41 .
  • the first solution contains tantalum.
  • the first solution is applied to a layer (a second material layer 420 ) exposed outside on a side of the first primary surface 21 of the electrically conductive substrate 2 .
  • the first condition includes a heat treatment temperature and a heat treatment time.
  • the heat treatment temperature (third prescribed temperature) of the first condition falls within a range of 100° C. to 400° C. for example, and the heat treatment temperature may be 220° C. as an example.
  • the heat treatment time of the first condition falls within a range of 5 minutes to 15 minutes for example, and the heat treatment time may be 10 minutes as an example.
  • the third process includes firing the stacked body 401 at a prescribed temperature (fourth prescribed temperature) to form the plurality of catalyst layers 42 and tantalum layers 41 , other than the tantalum layer 41 constituting the bottom layer, of the plurality of the tantalum layer 41 together with a plurality of cracks (recesses 5 ) recessed from a main surface 40 of the catalyst layer 42 .
  • the main surface 40 is a surface away from the intermediate layer 3 (see FIG. 7E ).
  • the first and second embodiments are only exemplary ones of various embodiments of the present disclosure.
  • the exemplary embodiment may be readily modified in various manners depending on a design choice or any other factor, as long as the purpose of the present disclosure can be attained.
  • the number of tantalum layers 41 and/or catalyst layers 42 of a composite layer 4 is not limited to four, but may be two, three, five or more.
  • the number of tantalum layers 41 and the number of catalyst layers 42 in the composite layer 4 are not limited to be the same, but may be different from each other.
  • thicknesses of a plurality of tantalum layers 41 are not limited to be the same, but may be different from each other. It is also possible that some of a plurality of tantalum layers 41 have the same thickness, and remaining of the plurality of tantalum layer 41 may have a thickness different therefrom.
  • thicknesses of a plurality of catalyst layers 42 are not limited to be the same, but may be different from each other. It is also possible that some of a plurality of catalyst layers 42 have the same thickness, and remaining of the plurality of catalyst layer 42 may have a thickness different therefrom.
  • a plurality of tantalum layers 41 are not limited to have the same composition, but may have different compositions.
  • a plurality of catalyst layers 42 are not limited to have the same composition, but may have different compositions.
  • each a plurality of catalyst layers 42 of a composite layer 4 is not limited to be a porous layer.
  • at least one catalyst layer 42 which is other than a catalyst layer 42 constituting a top layer of a plurality of catalyst layers 42 , may be a porous layer, for example.
  • each of a plurality of catalyst layers 42 of a composite layer 4 may be a non-porous layer.
  • a plurality of recesses 5 may have the same shape.
  • a method for producing such an electrode for electrolysis 1 may include an etching technique, a laser processing, or the like to form such a plurality of recesses 5 . These techniques/processing can provide a greater degree of freedom for the design of a layout and dimensions of the plurality of recesses 5 and can realize a higher reproductivity about the positions of the plurality of recesses 5 .
  • the electrode for electrolysis 1 b has a plurality of recesses 5 recessed from a main surface 40 , away from an intermediate layer 3 , of a composite layer 4 , and a top layer of the composite layer 4 is constituted by a tantalum layer 41 .
  • Components of the electrode for electrolysis 1 b similar to those of the electrode for electrolysis 1 are assigned same reference signs and explanation thereof may be omitted.
  • each of the plurality of recesses 5 has a depth such that each of the plurality of recesses 5 is made to go completely through at least one catalyst layer 42 of the plurality of catalyst layers 42 .
  • Each of the plurality of recesses 5 may preferably have a depth such that each of the plurality of recesses 5 is made to go completely through the plurality of catalyst layers 42 , which can contribute to improve the chlorine generation efficiency.
  • a bottom layer of a composite layer 4 may be constituted by one tantalum layer 41 of a plurality of tantalum layers 41 and be directly on a primary surface 21 of an electrically conductive substrate 2 without an intermediate layer 3 interposed therebetween.
  • a top layer, furthest from the electrically conductive substrate 2 , of the composite layer 4 may be constituted by one catalyst layer 42 of a plurality of catalyst layers 42 .
  • An electrode for electrolysis ( 1 ; 1 a ) includes an electrically conductive substrate ( 2 ), an intermediate layer ( 3 ), and a composite layer ( 4 ).
  • the electrically conductive substrate ( 2 ) contains at least titanium.
  • the intermediate layer ( 3 ) is provided on a primary surface ( 21 ) of the electrically conductive substrate ( 2 ).
  • the composite layer ( 4 ) is provided on the intermediate layer ( 3 ).
  • the composite layer ( 4 ) includes a plurality of tantalum layers ( 41 ) and a plurality of catalyst layers ( 42 ). Each of the plurality of tantalum layers ( 41 ) is made from tantalum oxide, tantalum, or a mixture of tantalum oxide and tantalum.
  • Each of the plurality of catalyst layers ( 42 ) contains platinum and iridium.
  • the plurality of tantalum layers ( 41 ) and the plurality of catalyst layers ( 42 ) are alternately stacked one layer by one layer in a thickness direction (D 1 ) of the electrically conductive substrate ( 2 ).
  • a bottom layer of the composite layer ( 4 ) closest to the primary surface ( 21 ) of the electrically conductive substrate ( 2 ) is constituted by one tantalum layer ( 41 ) of the plurality of tantalum layers ( 41 ).
  • a top layer of the composite layer ( 4 ) furthest from the electrically conductive substrate ( 2 ) is constituted by one catalyst layer ( 42 ) of the plurality of catalyst layers ( 42 ).
  • the electrode for electrolysis ( 1 ; 1 a ) according to the first aspect is less likely to cause the separation of the composite layer ( 4 ).
  • the electrode for electrolysis ( 1 ; 1 a ) according to a second aspect, which may be implemented in conjunction with the first aspect, the composite layer ( 4 ) has a main surface ( 40 ) away from the intermediate layer ( 3 ).
  • the electrode for electrolysis ( 1 ; 1 a ) has a plurality of recesses ( 5 ) recessed from the main surface ( 40 ) of the composite layer ( 4 ).
  • Each of the plurality of recesses ( 5 ) has a depth which is greater than a distance (L 1 ) between the main surface ( 40 ) of the composite layer ( 4 ) and a catalyst layer 42 (third catalyst layer 423 ), second furthest from the electrically conductive substrate ( 2 ), of the plurality of catalyst layers ( 42 ) and also is smaller than or equal to a distance (L 2 ) between the main surface ( 40 ) of the composite layer ( 4 ) and the intermediate layer ( 3 ).
  • a catalyst layer (third catalyst layer 423 ) second furthest from the electrically conductive substrate ( 2 ), of the plurality of catalyst layers ( 42 ), also can contribute to the generation of the chlorine.
  • the electrode for electrolysis ( 1 ; 1 a ) according to this aspect thus can contribute to improve the durability and also can achieve the efficient consumption of the catalyst layer ( 42 ) to improve the chlorine generation efficiency by adjusting at least one of the number of catalyst layers ( 42 ) and the percentage of iridium contained in each of the plurality of catalyst layers ( 42 ).
  • the electrode for electrolysis ( 1 a ) according to a third aspect, which may be implemented in conjunction with the second aspect, the depth of each of the plurality of recesses ( 5 ) is smaller than or equal to a distance (L 3 ) between the main surface ( 40 ) and the bottom layer (first tantalum layer 411 ) of the composite layer ( 4 ).
  • the electrode for electrolysis ( 1 a ) according to the third aspect is further less likely to cause the separation of the composite layer ( 4 ).
  • each of the plurality of recesses ( 5 ) is a crack extending linearly in a plan view as seen in the thickness direction (D 1 ).
  • a catalyst layer ( 42 ) farther from the electrically conductive substrate ( 2 ) tends to contribute to the generation of the chlorine and a catalyst layer ( 42 ) closer to the electrically conductive substrate ( 2 ) is less likely to be consumed. This can improve the durability of the electrode for electrolysis ( 1 ; 1 a ).
  • each of the plurality of recesses ( 5 ) has a width (H 1 ) within a range of 0.3 ⁇ m to 3 ⁇ m.
  • a percentage of S 2 with respect to S 1 +S 2 falls within a range of 5% to 50%, where S 1 denotes an area of the main surface ( 40 ) of the composite layer ( 4 ) in the plan view as seen in the thickness direction (D 1 ) of the electrically conductive substrate, and S 2 denotes a total area of opening areas of the plurality of recesses ( 5 ) in the main surface ( 40 ) of the composite layer ( 4 ) in the plan view as seen in the thickness direction (D 1 ) of the electrically conductive substrate.
  • the electrode for electrolysis ( 1 ; 1 a ) according to a seventh aspect, which may be implemented in conjunction with the sixth aspect, at least one recess ( 5 ) of the plurality of recesses ( 5 ) is present in a 0.01 mm 2 square region in the plan view as seen in the thickness direction (D 1 ) of the electrically conductive substrate ( 2 ), a total length of each opening edge of the at least one recess ( 5 ) present in the 0.01 mm 2 square region being greater than or equal to 1 mm.
  • each of the plurality of catalyst layers ( 42 ) is a porous layer.
  • the electrode for electrolysis ( 1 ; 1 a ) according to the eighth aspect can have an improved durability.
  • the reason that the electrode for electrolysis ( 1 ; 1 a ) according to the eighth aspect can have the improved durability may be inferred that each catalyst layer ( 42 ), other than a catalyst layer ( 42 ) that constitutes the top layer, of the plurality of catalyst layers ( 42 ) can easily contribute to generate the chlorine because the salt water is likely to infiltrate in an in-plane direction into the catalyst layer ( 42 ) through a side of this catalyst layer ( 42 ) exposed to the recess ( 5 ).
  • the electrode for electrolysis ( 1 ; 1 a ) according to a ninth aspect, which may be implemented in conjunction with any one of the first to eighth aspects, the primary surface ( 21 ) of the electrically conductive substrate ( 2 ) is uneven.
  • the electrode for electrolysis ( 1 ; 1 a ) according to the ninth aspect can improve the adhesion of the electrically conductive substrate ( 2 ) to the intermediate layer ( 3 ) and thus the composite layer ( 4 ) is less likely to be separated from the electrically conductive substrate ( 2 ).
  • a method for producing an electrode for electrolysis ( 1 a ) according to a tenth aspect includes an intermediate layer formation process and a composite layer formation process.
  • the intermediate layer formation process includes forming an intermediate layer ( 3 ) on a primary surface ( 21 ) of an electrically conductive substrate ( 2 ) containing titanium.
  • the composite layer formation process includes forming a composite layer ( 4 ) on the intermediate layer ( 3 ).
  • the composite layer ( 4 ) has a stacked structure alternating a plurality of tantalum layers ( 41 ) and a plurality of catalyst layers ( 42 ) one layer by one layer.
  • Each of the plurality of tantalum layers ( 41 ) is made from tantalum oxide, tantalum, or a mixture of tantalum oxide and tantalum.
  • the composite layer formation process includes a first process, a second process, and a third process.
  • the first process includes applying a solution containing tantalum onto the intermediate layer ( 3 ) and subsequently firing at a first prescribed temperature to form a tantalum layer ( 41 ), of the plurality of tantalum layers ( 41 ), that constitutes a bottom layer of the stacked structure.
  • the second process includes repeating a first step and a second step to form a stacked body ( 401 ) serving as a basis of a remaining part, other than the tantalum layer ( 41 ) that constitutes the bottom layer, of the stacked structure.
  • the third process includes firing the stacked body ( 401 ) at a fourth prescribed temperature, which is higher than each of the second prescribed temperature and the third prescribed temperature, to form the plurality of catalyst layers ( 42 ) and tantalum layers ( 41 ), other than the tantalum layer ( 41 ) that constitutes the bottom layer, of the plurality of tantalum layers ( 41 ) together with a plurality of cracks (recesses 5 ) recessed from a main surface ( 40 ) of the catalyst layer ( 42 ), the main surface ( 40 ) being a surface away from the intermediate layer ( 3 ).
  • the method for producing the electrode for electrolysis ( 1 a ) according to the tenth aspect is less likely to cause the separation of the composite layer ( 4 ).
  • the electrode for electrolysis ( 1 b ) according to the eleventh aspect is less likely to cause the separation of the composite layer ( 4 ).
  • An electrode for electrolysis ( 1 ; 1 a ) includes an electrically conductive substrate ( 2 ), an intermediate layer ( 3 ), and a composite layer ( 4 ).
  • the electrically conductive substrate ( 2 ) contains at least titanium.
  • the intermediate layer ( 3 ) is provided on a primary surface ( 21 ) of the electrically conductive substrate ( 2 ).
  • the composite layer ( 4 ) is provided on the intermediate layer ( 3 ).
  • the composite layer ( 4 ) includes a plurality of tantalum layers ( 41 ) and a plurality of catalyst layers ( 42 ). Each of the plurality of tantalum layers ( 41 ) is made from tantalum oxide, tantalum, or a mixture of tantalum oxide and tantalum.
  • the electrode for electrolysis ( 1 ; 1 a ) according to the twelfth aspect is less likely to cause the separation of the composite layer ( 4 ).

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  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
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