JPWO2023106412A5 - - Google Patents
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Claims (14)
導電性の第１の背面隔壁と、該第１の背面隔壁の外周部に設けられた第１のフランジ部と、前記第１の背面隔壁に電気的に接続された酸素発生用陽極とを備え、陽極室を画定する、陽極エンドセルと、
導電性の第２の背面隔壁と、該第２の背面隔壁の外周部に設けられた第２のフランジ部と、前記第２の背面隔壁に電気的に接続された水素発生用陰極とを備え、陰極室を画定する、陰極エンドセルと、
前記陽極エンドセルと前記陰極エンドセルとの間に配置され、それぞれイオン透過性の隔膜と、該隔膜の少なくとも周縁部を保持する保護部材とを備える、複数の隔膜要素と、
それぞれ導電性の第３の背面隔壁と、該第３の背面隔壁の外周部に設けられた第３のフランジ部と、前記第３の背面隔壁に電気的に接続された酸素発生用陽極とを備え、陽極室を画定する、複数の陽極室セルであって、該複数の陽極室セルのそれぞれは、それぞれの隣接する前記隔膜要素の間に配置されている、複数の陽極室セルと、
それぞれ導電性の第４の背面隔壁と、該第４の背面隔壁の外周部に設けられた第４のフランジ部と、前記第４の背面隔壁に電気的に接続された水素発生用陰極とを備え、陰極室を画定する、複数の陰極室セルであって、該複数の陰極室セルのそれぞれは、それぞれの隣接する前記隔膜要素の間に配置されている、複数の陰極室セルと、
を含む積層構造を備え、
それぞれの隣接する前記隔膜要素の間には、前記第３の背面隔壁を前記陽極エンドセル側に向けた一の陽極室セルと、前記第４の背面隔壁を前記陰極エンドセル側に向けた一の陰極室セルとの組が、該第３の背面隔壁と該第４の背面隔壁とが隣接するように配置され、
それぞれの隣接する前記隔膜要素の間において、前記第３の背面隔壁と前記第４の背面隔壁とは、一体に形成されていてもいなくてもよく、前記第３のフランジ部と前記第４のフランジ部とは、一体に形成されていてもいなくてもよく、
前記複数の隔膜要素は、前記陽極エンドセルに隣接する第１の隔膜要素と、前記陰極エンドセルに隣接する第２の隔膜要素とを含み、
前記陽極エンドセルの第１のフランジ部の下部、各陽極室セルの第３のフランジ部の下部、各陰極室セルの第４のフランジ部の下部、及び前記第２の隔膜要素以外の各隔膜要素の保護部材の下部には、陽極液供給用流通部が設けられており、
前記陰極エンドセルの第２のフランジ部の下部、及び前記第２の隔膜要素の保護部材の下部には、前記陽極液供給用流通部が設けられているか又は設けられておらず、
前記陽極エンドセル及び各陽極室セルのそれぞれは、前記陽極液供給用流通部および前記陽極室と流体連通して設けられた、陽極液供給用分岐流路を備え、
各陽極液供給用分岐流路を通じて、前記陽極液供給用流通部から各陽極室に陽極液が供給され、
前記陽極エンドセルの第１のフランジ部の上部、各陽極室セルの第３のフランジ部の上部、各陰極室セルの第４のフランジ部の上部、及び前記第２の隔膜要素以外の各隔膜要素の保護部材の上部には、陽極液・ガス回収用流通部が設けられており、
前記陰極エンドセルの第２のフランジ部の上部、及び前記第２の隔膜要素の保護部材の上部には、前記陽極液・ガス回収用流通部が設けられているか又は設けられておらず、
前記陽極エンドセル及び各陽極室セルのそれぞれは、前記陽極液・ガス回収用流通部および前記陽極室と流体連通して設けられた、陽極液・ガス回収用分岐流路を備え、
各陽極液・ガス回収用分岐流路を通じて、各陽極室から陽極液および陽極室中のガスが前記陽極液・ガス回収用流通部に回収され、
前記陰極エンドセルの第２のフランジ部の下部、各陽極室セルの第３のフランジ部の下部、各陰極室セルの第４のフランジ部の下部、及び前記第１の隔膜要素以外の各隔膜要素の保護部材の下部には、陰極液供給用流通部が設けられており、
前記陽極エンドセルの第１のフランジ部の下部、及び前記第１の隔膜要素の保護部材の下部には、前記陰極液供給用流通部が設けられているか又は設けられておらず、
前記陰極エンドセル及び各陰極室セルのそれぞれは、前記陰極液供給用流通部および前記陰極室と流体連通して設けられた、陰極液供給用分岐流路を備え、
各陰極液供給用分岐流路を通じて、前記陰極液供給用流通部から各陰極室に陰極液が供給され、
前記陰極エンドセルの第２のフランジ部の上部、各陽極室セルの第３のフランジ部の上部、各陰極室セルの第４のフランジ部の上部、及び前記第１の隔膜要素以外の各隔膜要素の保護部材の上部には、陰極液・ガス回収用流通部が設けられており、
前記陽極エンドセルの第１のフランジ部の上部、及び前記第１の隔膜要素の保護部材の上部には、前記陰極液・ガス回収用流通部が設けられているか又は設けられておらず、
前記陰極エンドセル及び各陰極室セルのそれぞれは、前記陰極液・ガス回収用流通部および前記陰極室と流体連通して設けられた、陰極液・ガス回収用分岐流路を備え、
各陰極液・ガス回収用分岐流路を通じて、各陰極室から陰極液および陰極室中のガスが前記陰極液・ガス回収用流通部に回収され、
前記陽極エンドセルの第１のフランジ部の、前記陽極液供給用流通部、前記陽極液供給用分岐流路、前記陽極液・ガス回収用流通部、及び前記陽極液・ガス回収用分岐流路に面した各表面の全部または一部が、それぞれ電気絶縁性の樹脂材料で覆われており、
前記陽極エンドセルの第１のフランジ部に前記陰極液供給用流通部が設けられている場合には、前記陽極エンドセルの第１のフランジ部の前記陰極液供給用流通部に面した表面の全部または一部が、電気絶縁性の樹脂材料で覆われており、
前記陽極エンドセルの第１のフランジ部に前記陰極液・ガス回収用流通部が設けられている場合には、前記陽極エンドセルの第１のフランジ部の前記陰極液・ガス回収用流通部に面した表面の全部または一部が、電気絶縁性の樹脂材料で覆われており、
前記陰極エンドセルの第２のフランジ部の、前記陰極液供給用流通部、前記陰極液供給用分岐流路、前記陰極液・ガス回収用流通部、及び前記陰極液・ガス回収用分岐流路に面した各表面の全部または一部が、それぞれ電気絶縁性の樹脂材料で覆われており、
前記陰極エンドセルの第２のフランジ部に前記陽極液供給用流通部が設けられている場合には、前記陰極エンドセルの第２のフランジ部の前記陽極液供給用流通部に面した表面の全部または一部が、電気絶縁性の樹脂材料で覆われており、
前記陰極エンドセルの第２のフランジ部に前記陽極液・ガス回収用流通部が設けられている場合には、前記陰極エンドセルの第２のフランジ部の前記陽極液・ガス回収用流通部に面した表面の全部または一部が、電気絶縁性の樹脂材料で覆われており、
前記陽極室セルの第３のフランジ部の、前記陽極液供給用流通部、前記陽極液供給用分岐流路、前記陽極液・ガス回収用流通部、前記陽極液・ガス回収用分岐流路、前記陰極液供給用流通部、及び前記陰極液・ガス回収用流通部に面した各表面の全部または一部が、それぞれ電気絶縁性の樹脂材料で覆われており、
前記陰極室セルの第４のフランジ部の、前記陰極液供給用流通部、前記陰極液供給用分岐流路、前記陰極液・ガス回収用流通部、前記陰極液・ガス回収用分岐流路、前記陽極液供給用流通部、及び前記陽極液・ガス回収用流通部に面した各表面の全部または一部が、それぞれ電気絶縁性の樹脂材料で覆われている
ことを特徴とし、
前記第３のフランジ部の、前記隔膜要素に接する表面の全部または一部が、電気絶縁性の樹脂材料で覆われており、
前記第４のフランジ部の、前記隔膜要素に接する表面の全部または一部が、電気絶縁性の樹脂材料で覆われている、
アルカリ水電解用電解槽。 An electrolytic cell for obtaining oxygen and hydrogen by electrolyzing an electrolytic solution consisting of alkaline water,
A conductive first back partition, a first flange provided on the outer periphery of the first back partition, and an oxygen generating anode electrically connected to the first back partition. , an anode end cell defining an anode chamber;
A conductive second back partition wall, a second flange portion provided on the outer periphery of the second back partition wall, and a hydrogen generation cathode electrically connected to the second back partition wall. , a cathode end cell defining a cathode chamber;
a plurality of diaphragm elements disposed between the anode end cell and the cathode end cell, each comprising an ion-permeable diaphragm and a protective member holding at least a peripheral edge of the diaphragm;
A conductive third back partition, a third flange provided on the outer periphery of the third back partition, and an oxygen generating anode electrically connected to the third back partition. a plurality of anode chamber cells defining an anode chamber, each of the plurality of anode chamber cells being disposed between respective adjacent membrane elements;
A fourth rear partition wall, each of which is electrically conductive, a fourth flange portion provided on the outer periphery of the fourth rear partition wall, and a hydrogen generation cathode electrically connected to the fourth rear partition wall. a plurality of cathode chamber cells defining a cathode chamber, each of the plurality of cathode chamber cells being disposed between respective adjacent said diaphragm elements;
Equipped with a laminated structure including
Between each of the adjacent diaphragm elements, there is provided one anode chamber cell with the third back partition facing the anode end cell side, and one cathode chamber cell with the fourth back partition facing the cathode end cell side. A set of chamber cells is arranged such that the third rear partition wall and the fourth rear partition wall are adjacent to each other,
Between each of the adjacent diaphragm elements, the third back partition and the fourth back partition may or may not be integrally formed, and the third flange and the fourth The flange portion may or may not be formed integrally.
The plurality of diaphragm elements include a first diaphragm element adjacent to the anode end cell and a second diaphragm element adjacent to the cathode end cell,
The lower part of the first flange part of the anode end cell, the lower part of the third flange part of each anode chamber cell, the lower part of the fourth flange part of each cathode chamber cell, and each diaphragm element other than the second diaphragm element. A flow section for anolyte supply is provided at the bottom of the protective member.
The anolyte supply flow part is provided or not provided at the lower part of the second flange part of the cathode end cell and the lower part of the protective member of the second diaphragm element,
Each of the anode end cell and each anode chamber cell includes an anolyte supply branch flow path provided in fluid communication with the anolyte supply flow section and the anode chamber,
The anolyte is supplied from the anolyte supply flow section to each anode chamber through each anolyte supply branch flow path,
The upper part of the first flange part of the anode end cell, the upper part of the third flange part of each anode chamber cell, the upper part of the fourth flange part of each cathode chamber cell, and each diaphragm element other than the second diaphragm element. The upper part of the protective member is equipped with a flow section for recovering the anolyte and gas.
The anolyte/gas recovery flow part is provided or not provided on the upper part of the second flange part of the cathode end cell and the upper part of the protective member of the second diaphragm element,
Each of the anode end cell and each anode chamber cell includes an anolyte/gas recovery branch flow path provided in fluid communication with the anolyte/gas recovery flow section and the anode chamber,
The anolyte and the gas in the anode chamber are collected from each anode chamber into the anolyte and gas recovery flow section through each anolyte and gas recovery branch flow path,
The lower part of the second flange part of the cathode end cell, the lower part of the third flange part of each anode chamber cell, the lower part of the fourth flange part of each cathode chamber cell, and each diaphragm element other than the first diaphragm element. A catholyte supply flow section is provided at the bottom of the protective member.
The catholyte supply flow part is provided or not provided at the lower part of the first flange part of the anode end cell and the lower part of the protective member of the first diaphragm element,
Each of the cathode end cell and each cathode chamber cell includes a catholyte supply branch flow path provided in fluid communication with the catholyte supply flow section and the cathode chamber,
The catholyte is supplied from the catholyte supply flow section to each cathode chamber through each catholyte supply branch flow path,
The upper part of the second flange part of the cathode end cell, the upper part of the third flange part of each anode chamber cell, the upper part of the fourth flange part of each cathode chamber cell, and each diaphragm element other than the first diaphragm element. A catholyte/gas recovery circulation section is provided at the top of the protective member.
The catholyte/gas recovery circulation part is provided or not provided in the upper part of the first flange part of the anode end cell and the upper part of the protective member of the first diaphragm element,
Each of the cathode end cell and each cathode chamber cell includes a catholyte/gas recovery branch flow path provided in fluid communication with the catholyte/gas recovery flow section and the cathode chamber,
The catholyte and the gas in the cathode chamber are collected from each catholyte chamber into the catholyte and gas recovery flow section through each catholyte and gas recovery branch flow path,
The anolyte supply flow section, the anolyte supply branch flow path, the anolyte/gas recovery flow section, and the anolyte/gas recovery branch flow path of the first flange portion of the anode end cell. All or part of each facing surface is covered with an electrically insulating resin material,
When the catholyte supply flow section is provided in the first flange section of the anode end cell, the entire surface of the first flange section of the anode end cell facing the catholyte supply flow section or A portion is covered with an electrically insulating resin material,
When the catholyte/gas recovery circulation part is provided in the first flange part of the anode end cell, the catholyte/gas recovery circulation part of the first flange part of the anode end cell faces the catholyte/gas recovery circulation part. All or part of the surface is covered with an electrically insulating resin material,
In the second flange part of the cathode end cell, the catholyte supply flow section, the catholyte supply branch flow path, the catholyte/gas recovery flow section, and the catholyte/gas recovery branch flow path. All or part of each facing surface is covered with an electrically insulating resin material,
When the second flange portion of the cathode end cell is provided with the anolyte supply flow portion, the entire surface of the second flange portion of the cathode end cell facing the anolyte supply flow portion or A portion is covered with an electrically insulating resin material,
When the anolyte/gas recovery flow section is provided in the second flange section of the cathode end cell, the second flange section of the cathode end cell facing the anolyte/gas recovery flow section All or part of the surface is covered with an electrically insulating resin material,
the anolyte supply flow section, the anolyte supply branch flow path, the anolyte/gas recovery flow section, the anolyte/gas recovery branch flow path of the third flange portion of the anode chamber cell; All or part of each surface facing the catholyte supply flow section and the catholyte/gas recovery flow section is covered with an electrically insulating resin material,
the catholyte supply flow section, the catholyte supply branch flow path, the catholyte/gas recovery flow section, the catholyte/gas recovery branch flow path of the fourth flange portion of the catholyte chamber cell; All or part of each surface facing the anolyte supply flow section and the anolyte/gas recovery flow section is covered with an electrically insulating resin material,
All or part of the surface of the third flange portion that is in contact with the diaphragm element is covered with an electrically insulating resin material,
All or part of the surface of the fourth flange portion that is in contact with the diaphragm element is covered with an electrically insulating resin material.
Electrolyzer for alkaline water electrolysis.
各陽極室セルは、
前記第３のフランジ部の下部を積層方向に貫通して設けられた、陽極液供給用流通孔および陰極液供給用流通孔と、
前記第３のフランジ部の上部を積層方向に貫通して設けられた、陽極液・ガス回収用流通孔および陰極液・ガス回収用流通孔と、
を備え、
前記陽極室セルに設けられた前記陽極液供給用分岐流路は、該陽極室セルが画定する陽極室と、該陽極室セルに設けられた前記陽極液供給用流通孔とに流体連通して設けられており、
前記陽極室セルに設けられた前記陽極液・ガス回収用分岐流路は、該陽極室セルが画定する陽極室と、該陽極室セルに設けられた前記陽極液・ガス回収用流通孔とに流体連通して設けられており、
各陰極室セルは、
前記第４のフランジ部の下部を積層方向に貫通して設けられた、陽極液供給用流通孔および陰極液供給用流通孔と、
前記第４のフランジ部の上部を積層方向に貫通して設けられた、陽極液・ガス回収用流通孔および陰極液・ガス回収用流通孔と、
を備え、
前記陰極室セルに設けられた前記陰極液供給用分岐流路は、該陰極室セルが画定する陰極室と、該陰極室セルに設けられた前記陰極液供給用流通孔とに流体連通して設けられており、
前記陰極室セルに設けられた前記陰極液・ガス回収用分岐流路は、該陰極室セルが画定する陰極室と、該陰極室セルに設けられた前記陰極液・ガス回収用流通孔とに流体連通して設けられており、
前記第１の隔膜要素および前記第２の隔膜要素以外の各隔膜要素は、
前記保護部材の下部を積層方向に貫通して設けられた、陽極液供給用流通孔および陰極液供給用流通孔と、
前記保護部材の上部を積層方向に貫通して設けられた、陽極液・ガス回収用流通孔および陰極液・ガス回収用流通孔と、
を備え、
前記第１の隔膜要素は、
前記保護部材の下部を積層方向に貫通して設けられた、陽極液供給用流通孔と、
前記保護部材の上部を積層方向に貫通して設けられた、陽極液・ガス回収用流通孔と、
を備え、
前記陽極エンドセルの第１のフランジ部に前記陰極液供給用流通部が設けられている場合には、前記第１の隔膜要素の保護部材は、該保護部材の下部を積層方向に貫通して設けられた陰極液供給用流通孔をさらに備え、
前記陽極エンドセルの第１のフランジ部に前記陰極液・ガス回収用流通部が設けられている場合には、前記第１の隔膜要素の保護部材は、該保護部材の下部を積層方向に貫通して設けられた陰極液・ガス回収用流通孔をさらに備え、
前記第２の隔膜要素は、
前記保護部材の下部を積層方向に貫通して設けられた、陰極液供給用流通孔と、
前記保護部材の上部を積層方向に貫通して設けられた、陰極液・ガス回収用流通孔と、
を備え、
前記陰極エンドセルの第２のフランジ部に前記陽極液供給用流通部が設けられている場合には、前記第２の隔膜要素の保護部材は、該保護部材の下部を積層方向に貫通して設けられた陽極液供給用流通孔をさらに備え、
前記陰極エンドセルの第２のフランジ部に前記陽極液・ガス回収用流通部が設けられている場合には、前記第２の隔膜要素の保護部材は、該保護部材の上部を積層方向に貫通して設けられた陽極液・ガス回収用流通孔をさらに備え、
前記複数の陽極室セルに設けられた各陽極液供給用流通孔と、前記複数の陰極室セルに設けられた各陽極液供給用流通孔と、前記複数の隔膜要素に設けられた各陽極液供給用流通孔とが流体連通することにより形成された一体の連続した陽極液供給用流通部が、前記陽極エンドセルの陽極液供給用流通部、および、前記陰極エンドセルに陽極液供給用流通部が設けられている場合には該陰極エンドセルの陽極液供給用流通部と、さらに流体連通しており、
前記複数の陽極室セルに設けられた各陽極液・ガス回収用流通孔と、前記複数の陰極室セルに設けられた各陽極液・ガス回収用流通孔と、前記複数の隔膜要素に設けられた各陽極液・ガス回収用流通孔とが流体連通することにより形成された一体の連続した陽極液・ガス回収用流通部が、前記陽極エンドセルの陽極液・ガス回収用流通部、および、前記陰極エンドセルに陽極液・ガス回収用流通部が設けられている場合には該陰極エンドセルの陽極液・ガス回収用流通部と、さらに流体連通しており、
前記複数の陽極室セルに設けられた各陰極液供給用流通孔と、前記複数の陰極室セルに設けられた各陰極液供給用流通孔と、前記複数の隔膜要素に設けられた各陰極液供給用流通孔とが流体連通することにより形成された一体の連続した陰極液供給用流通部が、前記陰極エンドセルの陰極液供給用流通部、および、前記陽極エンドセルに陰極液供給用流通部が設けられている場合には該陽極エンドセルの陰極液供給用流通部と、さらに流体連通しており、
前記複数の陽極室セルに設けられた各陰極液・ガス回収用流通孔と、前記複数の陰極室セルに設けられた各陰極液・ガス回収用流通孔と、前記複数の隔膜要素に設けられた各陰極液・ガス回収用流通孔とが流体連通することにより形成された一体の連続した陰極液・ガス回収用流通部が、前記陰極エンドセルの陰極液・ガス回収用流通部、および、前記陽極エンドセルに陰極液・ガス回収用流通部が設けられている場合には該陽極エンドセルの陰極液・ガス回収用流通部と、さらに流体連通しており、
各陽極室セルの第３のフランジ部の、前記陽極液供給用流通孔、前記陰極液供給用流通孔、前記陽極液・ガス回収用流通孔、前記陰極液・ガス回収用流通孔、前記陽極液供給用分岐流路、及び前記陽極液・ガス回収用分岐流路に面した各表面の全部または一部が、それぞれ電気絶縁性の樹脂材料で覆われており、
各陰極室セルの第４のフランジ部の、前記陽極液供給用流通孔、前記陰極液供給用流通孔、前記陽極液・ガス回収用流通孔、前記陰極液・ガス回収用流通孔、前記陰極液供給用分岐流路、及び前記陰極液・ガス回収用分岐流路に面した各表面の全部または一部が、それぞれ電気絶縁性の樹脂材料で覆われている、
請求項１に記載の電解槽。 Between each of the adjacent diaphragm elements, the third back partition wall and the fourth back partition wall are not integrally formed, and the third flange portion and the fourth flange portion are integrally formed. the anode chamber cell and the cathode chamber cell are separate electrolytic cells;
Each anode chamber cell is
an anolyte supply flow hole and a catholyte supply flow hole provided to penetrate the lower part of the third flange portion in the stacking direction;
An anolyte/gas recovery communication hole and a catholyte/gas recovery communication hole provided to penetrate the upper part of the third flange portion in the stacking direction;
Equipped with
The anolyte supply branch flow path provided in the anode chamber cell is in fluid communication with an anode chamber defined by the anode chamber cell and the anolyte supply flow hole provided in the anode chamber cell. It is provided,
The anolyte/gas recovery branch flow path provided in the anode chamber cell is connected to the anode chamber defined by the anode chamber cell and the anolyte/gas recovery flow hole provided in the anode chamber cell. provided in fluid communication;
Each cathode chamber cell is
an anolyte supply flow hole and a catholyte supply flow hole provided to penetrate the lower part of the fourth flange portion in the stacking direction;
An anolyte/gas recovery communication hole and a catholyte/gas recovery communication hole provided to penetrate the upper part of the fourth flange portion in the stacking direction;
Equipped with
The catholyte supply branch channel provided in the cathode chamber cell is in fluid communication with a cathode chamber defined by the cathode chamber cell and the catholyte supply flow hole provided in the cathode chamber cell. It is provided,
The catholyte/gas recovery branch flow path provided in the cathode chamber cell is connected to the cathode chamber defined by the cathode chamber cell and the catholyte/gas recovery circulation hole provided in the cathode chamber cell. provided in fluid communication;
Each diaphragm element other than the first diaphragm element and the second diaphragm element is
an anolyte supply flow hole and a catholyte supply flow hole provided to penetrate the lower part of the protective member in the stacking direction;
an anolyte/gas recovery circulation hole and a catholyte/gas recovery circulation hole provided through the upper part of the protective member in the stacking direction;
Equipped with
The first diaphragm element is
an anolyte supply flow hole provided through the lower part of the protective member in the stacking direction;
an anolyte/gas recovery flow hole provided through the upper part of the protective member in the stacking direction;
Equipped with
When the catholyte supply flow section is provided in the first flange portion of the anode end cell, the protective member of the first diaphragm element is provided so as to penetrate through the lower part of the protective member in the stacking direction. further comprising a catholyte supplying passage hole,
When the catholyte/gas recovery flow section is provided in the first flange portion of the anode end cell, the protective member of the first diaphragm element penetrates the lower part of the protective member in the stacking direction. It is further equipped with a catholyte and gas recovery circulation hole,
The second diaphragm element is
a catholyte supply circulation hole provided through the lower part of the protective member in the stacking direction;
a catholyte/gas recovery circulation hole provided through the upper part of the protective member in the stacking direction;
Equipped with
When the anolyte supply flow section is provided in the second flange portion of the cathode end cell, the protective member of the second diaphragm element is provided so as to penetrate through the lower part of the protective member in the stacking direction. It further includes a flow hole for supplying the anolyte,
When the anolyte/gas recovery flow section is provided in the second flange portion of the cathode end cell, the protective member of the second diaphragm element passes through the upper part of the protective member in the stacking direction. It is further equipped with anolyte and gas recovery flow holes provided in the
Each anolyte supply flow hole provided in the plurality of anode chamber cells, each anolyte supply flow hole provided in the plurality of cathode chamber cells, and each anolyte solution provided in the plurality of diaphragm elements. An integrated continuous anolyte supply flow section formed by fluid communication with the supply flow hole is an anolyte supply flow section of the anode end cell, and an anolyte supply flow section of the cathode end cell. if provided, further in fluid communication with the anolyte supply flow section of the cathode end cell;
Each anolyte/gas recovery circulation hole provided in the plurality of anode chamber cells, each anolyte/gas recovery circulation hole provided in the plurality of cathode chamber cells, and each anolyte/gas recovery circulation hole provided in the plurality of diaphragm elements. An integral continuous anolyte/gas recovery flow section formed by fluidly communicating the anolyte/gas recovery flow holes of the anode end cell, and the anolyte/gas recovery flow section of the anode end cell, If the cathode end cell is provided with an anolyte/gas recovery circulation section, it is further in fluid communication with the anolyte/gas recovery circulation section of the cathode end cell;
Each catholyte supply communication hole provided in the plurality of anode chamber cells, each catholyte supply communication hole provided in the plurality of cathode chamber cells, and each catholyte solution provided in the plurality of diaphragm elements. An integrated continuous catholyte supply flow section formed by fluid communication with the supply flow hole is a catholyte supply flow section in the cathode end cell, and a catholyte supply flow section in the anode end cell. If provided, it is further in fluid communication with the catholyte supply flow section of the anode end cell,
Each catholyte/gas recovery circulation hole provided in the plurality of anode chamber cells, each catholyte/gas recovery circulation hole provided in the plurality of cathode chamber cells, and each catholyte/gas recovery circulation hole provided in the plurality of diaphragm elements. An integrated and continuous catholyte/gas recovery circulation section formed by fluidly communicating each of the catholyte/gas recovery circulation holes is connected to the catholyte/gas recovery circulation section of the cathode end cell, and the catholyte/gas recovery circulation section of the cathode end cell. If the anode end cell is provided with a catholyte/gas recovery circulation section, it is further in fluid communication with the catholyte/gas recovery circulation section of the anode end cell;
The anolyte supply flow hole, the catholyte supply flow hole, the anolyte/gas recovery flow hole, the catholyte/gas recovery flow hole, and the anode of the third flange portion of each anode chamber cell. All or part of each surface facing the liquid supply branch channel and the anolyte/gas recovery branch channel is covered with an electrically insulating resin material,
The anolyte supply flow hole, the catholyte supply flow hole, the anolyte/gas recovery flow hole, the catholyte/gas recovery flow hole, and the cathode in the fourth flange portion of each cathode chamber cell. All or part of each surface facing the liquid supply branch channel and the catholyte/gas recovery branch channel is covered with an electrically insulating resin material, respectively.
The electrolytic cell according to claim 1.
各バイポーラ電解エレメントは、
前記第３のフランジ部および前記第４のフランジ部の下部を積層方向に貫通して設けられた、陽極液供給用流通孔および陰極液供給用流通孔と、
前記第３のフランジ部および前記第４のフランジ部の上部を積層方向に貫通して設けられた、陽極液・ガス回収用流通孔および陰極液・ガス回収用流通孔と、
を備え、
各バイポーラ電解エレメントの陽極液供給用分岐流路は、該バイポーラ電解エレメントが画定する陽極室と、該バイポーラ電解エレメントに設けられた前記陽極液供給用流通孔とに流体連通して設けられており、
各バイポーラ電解エレメントの陽極液・ガス回収用分岐流路は、該バイポーラ電解エレメントが画定する陽極室と、該バイポーラ電解エレメントに設けられた前記陽極液・ガス回収用流通孔とに流体連通して設けられており、
各バイポーラ電解エレメントの陰極液供給用分岐流路は、該バイポーラ電解エレメントが画定する陰極室と、該バイポーラ電解エレメントに設けられた前記陰極液供給用流通孔とに流体連通して設けられており、
各バイポーラ電解エレメントの陰極液・ガス回収用分岐流路は、該バイポーラ電解エレメントが画定する陰極室と、該バイポーラ電解エレメントに設けられた前記陰極液・ガス回収用流通孔とに流体連通して設けられており、
前記第１の隔膜要素および前記第２の隔膜要素以外の各隔膜要素は、
前記保護部材の下部を積層方向に貫通して設けられた、陽極液供給用流通孔および陰極液供給用流通孔と、
前記保護部材の上部を積層方向に貫通して設けられた、陽極液・ガス回収用流通孔および陰極液・ガス回収用流通孔と、
を備え、
前記第１の隔膜要素は、
前記保護部材の下部を積層方向に貫通して設けられた、陽極液供給用流通孔と、
前記保護部材の上部を積層方向に貫通して設けられた、陽極液・ガス回収用流通孔と、
を備え、
前記陽極エンドセルの第１のフランジ部に前記陰極液供給用流通部が設けられている場合には、前記第１の隔膜要素の保護部材は、該保護部材の下部を積層方向に貫通して設けられた陰極液供給用流通孔をさらに備え、
前記陽極エンドセルの第１のフランジ部に前記陰極液・ガス回収用流通部が設けられている場合には、前記第１の隔膜要素の保護部材は、該保護部材の下部を積層方向に貫通して設けられた陰極液・ガス回収用流通孔をさらに備え、
前記第２の隔膜要素は、
前記保護部材の下部を積層方向に貫通して設けられた、陰極液供給用流通孔と、
前記保護部材の上部を積層方向に貫通して設けられた、陰極液・ガス回収用流通孔と、
を備え、
前記陰極エンドセルの第２のフランジ部に前記陽極液供給用流通部が設けられている場合には、前記第２の隔膜要素の保護部材は、該保護部材の下部を積層方向に貫通して設けられた陽極液供給用流通孔をさらに備え、
前記陰極エンドセルの第２のフランジ部に前記陽極液・ガス回収用流通部が設けられている場合には、前記第２の隔膜要素の保護部材は、該保護部材の上部を積層方向に貫通して設けられた陽極液・ガス回収用流通孔をさらに備え、
各バイポーラ電解エレメントに設けられた陽極液供給用流通孔と、前記複数の隔膜要素に設けられた各陽極液供給用流通孔とが流体連通することにより形成された一体の連続した陽極液供給用流通部が、前記陽極エンドセルの陽極液供給用流通部、および、前記陰極エンドセルに陽極液供給用流通部が設けられている場合には該陰極エンドセルの陽極液供給用流通部と、さらに流体連通しており、
各バイポーラ電解エレメントに設けられた陽極液・ガス回収用流通孔と、前記複数の隔膜要素に設けられた各陽極液・ガス回収用流通孔とが流体連通することにより形成された一体の連続した陽極液・ガス回収用流通部が、前記陽極エンドセルの陽極液・ガス回収用流通部、および、前記陰極エンドセルに陽極液・ガス回収用流通部が設けられている場合には該陰極エンドセルの陽極液・ガス回収用流通部と、さらに流体連通しており、
各バイポーラ電解エレメントに設けられた陰極液供給用流通孔と、前記複数の隔膜要素に設けられた各陰極液供給用流通孔とが流体連通することにより形成された一体の連続した陰極液供給用流通部が、前記陰極エンドセルの陰極液供給用流通部、および、前記陽極エンドセルに陰極液供給用流通部が設けられている場合には該陽極エンドセルの陰極液供給用流通部と、さらに流体連通しており、
各バイポーラ電解エレメントに設けられた陰極液・ガス回収用流通孔と、前記複数の隔膜要素に設けられた各陰極液・ガス回収用流通孔とが流体連通することにより形成された一体の連続した陰極液・ガス回収用流通部が、前記陰極エンドセルの陰極液・ガス回収用流通部、および、前記陽極エンドセルに陰極液・ガス回収用流通部が設けられている場合には該陽極エンドセルの陰極液・ガス回収用流通部と、さらに流体連通しており、
各バイポーラ電解エレメントの第３のフランジ部および第４のフランジ部の、陽極液供給用流通孔、陰極液供給用流通孔、陽極液・ガス回収用流通孔、陰極液・ガス回収用流通孔、陽極液供給用分岐流路、陰極液供給用分岐流路、陽極液・ガス回収用分岐流路、及び陰極液・ガス回収用分岐流路に面した各表面の全部または一部が、それぞれ電気絶縁性の樹脂材料で覆われている、
請求項１に記載の電解槽。 The third rear partition wall and the fourth rear partition wall are formed as an integral partition wall between the adjacent partition elements, and the third flange portion and the fourth flange portion are formed as an integral partition wall. are integrally formed, and the set of the anode chamber cell and the cathode chamber cell constitutes a single bipolar electrolytic element,
Each bipolar electrolytic element is
an anolyte supply flow hole and a catholyte supply flow hole provided to penetrate the lower portions of the third flange portion and the fourth flange portion in the stacking direction;
An anolyte/gas recovery flow hole and a catholyte/gas recovery flow hole provided to penetrate the upper portions of the third flange portion and the fourth flange portion in the stacking direction;
Equipped with
The anolyte supply branch channel of each bipolar electrolysis element is provided in fluid communication with the anode chamber defined by the bipolar electrolysis element and the anolyte supply flow hole provided in the bipolar electrolysis element. ,
The anolyte/gas recovery branch channel of each bipolar electrolysis element is in fluid communication with the anode chamber defined by the bipolar electrolysis element and the anolyte/gas recovery flow hole provided in the bipolar electrolysis element. It is provided,
The catholyte supply branch channel of each bipolar electrolytic element is provided in fluid communication with the cathode chamber defined by the bipolar electrolytic element and the catholyte supply circulation hole provided in the bipolar electrolytic element. ,
The catholyte/gas recovery branch channel of each bipolar electrolytic element is in fluid communication with the cathode chamber defined by the bipolar electrolytic element and the catholyte/gas recovery circulation hole provided in the bipolar electrolytic element. It is provided,
Each diaphragm element other than the first diaphragm element and the second diaphragm element is
an anolyte supply flow hole and a catholyte supply flow hole provided to penetrate the lower part of the protective member in the stacking direction;
an anolyte/gas recovery circulation hole and a catholyte/gas recovery circulation hole provided through the upper part of the protective member in the stacking direction;
Equipped with
The first diaphragm element is
an anolyte supply flow hole provided through the lower part of the protective member in the stacking direction;
an anolyte/gas recovery flow hole provided through the upper part of the protective member in the stacking direction;
Equipped with
When the catholyte supply flow section is provided in the first flange portion of the anode end cell, the protective member of the first diaphragm element is provided so as to penetrate through the lower part of the protective member in the stacking direction. further comprising a catholyte supplying passage hole,
When the catholyte/gas recovery flow section is provided in the first flange portion of the anode end cell, the protective member of the first diaphragm element penetrates the lower part of the protective member in the stacking direction. It is further equipped with a catholyte and gas recovery circulation hole,
The second diaphragm element is
a catholyte supply circulation hole provided through the lower part of the protective member in the stacking direction;
a catholyte/gas recovery circulation hole provided through the upper part of the protective member in the stacking direction;
Equipped with
When the anolyte supply flow section is provided in the second flange portion of the cathode end cell, the protective member of the second diaphragm element is provided so as to penetrate through the lower part of the protective member in the stacking direction. It further includes a flow hole for supplying the anolyte,
When the anolyte/gas recovery flow section is provided in the second flange portion of the cathode end cell, the protective member of the second diaphragm element passes through the upper part of the protective member in the stacking direction. It is further equipped with anolyte and gas recovery flow holes provided in the
An integrated continuous anolyte supply system formed by fluidly communicating the anolyte supply flow hole provided in each bipolar electrolytic element with each anolyte supply flow hole provided in the plurality of diaphragm elements. The flow section is in fluid communication with the anolyte supply flow section of the anode end cell and, if the cathode end cell is provided with an anolyte supply flow section, with the anolyte supply flow section of the cathode end cell. and
An integrated, continuous system formed by fluidly communicating the anolyte/gas recovery holes provided in each bipolar electrolytic element with the anolyte/gas recovery holes provided in the plurality of diaphragm elements. The anolyte/gas recovery circulation section is the anolyte/gas recovery circulation section of the anode end cell, and if the cathode end cell is provided with the anolyte/gas recovery circulation section, the anode of the cathode end cell. It is also in fluid communication with the liquid/gas recovery distribution section.
A continuous catholyte supply system formed by fluidly communicating a catholyte supply flow hole provided in each bipolar electrolytic element with each catholyte supply flow hole provided in the plurality of diaphragm elements. The flow section is in fluid communication with the catholyte supply flow section of the cathode end cell and, if the catholyte supply flow section is provided in the anode end cell, with the catholyte supply flow section of the anode end cell. and
An integral continuous system formed by fluid communication between the catholyte/gas recovery circulation holes provided in each bipolar electrolytic element and each catholyte/gas recovery circulation hole provided in the plurality of diaphragm elements. The catholyte/gas recovery flow section is the catholyte/gas recovery flow section of the cathode end cell, and if the catholyte/gas recovery flow section is provided in the anode end cell, the cathode of the anode end cell. It is also in fluid communication with the liquid/gas recovery distribution section.
Anolyte supply flow holes, catholyte supply flow holes, anolyte/gas recovery flow holes, catholyte/gas recovery flow holes in the third flange portion and fourth flange portion of each bipolar electrolytic element; All or part of each surface facing the branch channel for anolyte supply, branch channel for catholyte supply, branch channel for anolyte/gas recovery, and branch channel for catholyte/gas recovery is electrically connected. covered with insulating resin material,
The electrolytic cell according to claim 1.
前記陽極エンドセルの第１のフランジ部に前記陰極液供給用流通部が設けられている場合には、前記陽極エンドセルの第１のフランジ部の前記陰極液供給用流通部に面した表面の面積の９９．０％以上が、前記電気絶縁性の樹脂材料で覆われており、
前記陽極エンドセルの第１のフランジ部に前記陰極液・ガス回収用流通部が設けられている場合には、前記陽極エンドセルの第１のフランジ部の前記陰極液・ガス回収用流通部に面した表面の面積の９９．０％以上が、前記電気絶縁性の樹脂材料で覆われており、
前記陰極エンドセルの第２のフランジ部の、前記陰極液供給用流通部、前記陰極液供給用分岐流路、前記陰極液・ガス回収用流通部、及び前記陰極液・ガス回収用分岐流路に面した各表面の面積の９９．０％以上が、それぞれ前記電気絶縁性の樹脂材料で覆われており、
前記陰極エンドセルの第２のフランジ部に前記陽極液供給用流通部が設けられている場合には、前記陰極エンドセルの第２のフランジ部の前記陽極液供給用流通部に面した表面の面積の９９．０％以上が、前記電気絶縁性の樹脂材料で覆われており、
前記陰極エンドセルの第２のフランジ部に前記陽極液・ガス回収用流通部が設けられている場合には、前記陰極エンドセルの第２のフランジ部の前記陽極液・ガス回収用流通部に面した表面の面積の９９．０％以上が、前記電気絶縁性の樹脂材料で覆われており、
前記第３のフランジ部の、前記陽極液供給用流通部、前記陽極液供給用分岐流路、前記陽極液・ガス回収用流通部、前記陽極液・ガス回収用分岐流路、前記陰極液供給用流通部、及び前記陰極液・ガス回収用流通部に面した各表面の面積の９９．０％以上が、それぞれ前記電気絶縁性の樹脂材料で覆われており、
前記第４のフランジ部の、前記陰極液供給用流通部、前記陰極液供給用分岐流路、前記陰極液・ガス回収用流通部、前記陰極液・ガス回収用分岐流路、前記陽極液供給用流通部、及び前記陽極液・ガス回収用流通部に面した各表面の面積の９９．０％以上が、それぞれ前記電気絶縁性の樹脂材料で覆われている、
請求項１～３のいずれかに記載の電解槽。 The anolyte supply flow section, the anolyte supply branch flow path, the anolyte/gas recovery flow section, and the anolyte/gas recovery branch flow path of the first flange portion of the anode end cell. 99.0% or more of the area of each facing surface is covered with the electrically insulating resin material,
When the catholyte supply flow section is provided in the first flange section of the anode end cell, the area of the surface of the first flange section of the anode end cell facing the catholyte supply flow section is 99.0% or more is covered with the electrically insulating resin material,
When the catholyte/gas recovery circulation part is provided in the first flange part of the anode end cell, the catholyte/gas recovery circulation part of the first flange part of the anode end cell faces the catholyte/gas recovery circulation part. 99.0% or more of the surface area is covered with the electrically insulating resin material,
In the second flange part of the cathode end cell, the catholyte supply flow section, the catholyte supply branch flow path, the catholyte/gas recovery flow section, and the catholyte/gas recovery branch flow path. 99.0% or more of the area of each facing surface is covered with the electrically insulating resin material,
When the second flange portion of the cathode end cell is provided with the anolyte supply flow portion, the area of the surface of the second flange portion of the cathode end cell facing the anolyte supply flow portion is 99.0% or more is covered with the electrically insulating resin material,
When the anolyte/gas recovery flow section is provided in the second flange section of the cathode end cell, the second flange section of the cathode end cell facing the anolyte/gas recovery flow section 99.0% or more of the surface area is covered with the electrically insulating resin material,
The anolyte supply flow section, the anolyte supply branch flow path, the anolyte/gas recovery flow section, the anolyte/gas recovery branch flow path, and the catholyte supply of the third flange portion. 99.0% or more of the area of each surface facing the communication flow section and the catholyte/gas recovery flow section is covered with the electrically insulating resin material, respectively;
The catholyte supply distribution section, the catholyte supply branch flow path, the catholyte/gas recovery distribution section, the catholyte/gas recovery branch flow path, and the anolyte supply of the fourth flange portion. 99.0% or more of the area of each surface facing the anolyte/gas recovery circulation section and the anolyte/gas recovery circulation section is covered with the electrically insulating resin material, respectively.
The electrolytic cell according to any one of claims 1 to 3.
前記第４のフランジ部の、前記隔膜要素に接する表面の面積の９９．０％以上が、電気絶縁性の樹脂材料で覆われている、
請求項１～３に記載の電解槽。 99.0% or more of the surface area of the third flange portion in contact with the diaphragm element is covered with an electrically insulating resin material,
99.0% or more of the surface area of the fourth flange portion in contact with the diaphragm element is covered with an electrically insulating resin material;
The electrolytic cell according to claims 1 to 3 .
請求項１～３のいずれかに記載の電解槽。 On each surface covered with the electrically insulating resin material, the thickness of the coating with the electrically insulating resin material is 50 to 1500 μm.
The electrolytic cell according to any one of claims 1 to 3.
前記陰極液供給用流通部が、前記第１の隔膜要素の保護部材の下部および前記陽極エンドセルの第１のフランジ部の下部にも、該第１のフランジ部を貫通して設けられており、
前記陰極液・ガス回収用流通部が、前記第１の隔膜要素の保護部材の上部および前記陽極エンドセルの第１のフランジ部の上部にも、該第１のフランジ部を貫通して設けられており、
前記陽極エンドセルに設けられた前記陽極液供給用流通部を通じて、前記電解槽の外部から陽極液が各陽極室に供給され、
前記陽極エンドセルに設けられた前記陰極液供給用流通部を通じて、前記電解槽の外部から陰極液が各陰極室に供給され、
前記陽極エンドセルに設けられた前記陽極液・ガス回収用流通部を通じて、陽極液および各陽極室中のガスが、各陽極室から前記電解槽の外部に取り出され、
前記陽極エンドセルに設けられた前記陰極液・ガス回収用流通部を通じて、陰極液および各陰極室中のガスが、各陰極室から前記電解槽の外部に取り出される、
請求項１～３のいずれかに記載の電解槽。 The anolyte supply flow part and the anolyte/gas recovery flow part are provided to penetrate the first flange part of the anode end cell,
The catholyte supply flow section is also provided at a lower part of the protective member of the first diaphragm element and a lower part of the first flange part of the anode end cell, penetrating the first flange part,
The catholyte/gas recovery flow section is also provided above the protective member of the first diaphragm element and above the first flange section of the anode end cell, penetrating the first flange section. Ori,
An anolyte is supplied to each anode chamber from outside the electrolytic cell through the anolyte supply flow section provided in the anode end cell,
A catholyte is supplied from the outside of the electrolytic cell to each cathode chamber through the catholyte supply flow section provided in the anode end cell,
The anolyte and the gas in each anode chamber are taken out from each anode chamber to the outside of the electrolytic cell through the anolyte/gas recovery flow section provided in the anode end cell,
The catholyte and the gas in each cathode chamber are taken out from each cathode chamber to the outside of the electrolytic cell through the catholyte/gas recovery circulation section provided in the anode end cell.
The electrolytic cell according to any one of claims 1 to 3.
前記陽極液供給用流通部が、前記第２の隔膜要素の保護部材の下部および前記陰極エンドセルの第２のフランジ部の下部にも、該第２のフランジ部を貫通して設けられており、
前記陽極液・ガス回収用流通部が、前記第２の隔膜要素の保護部材の上部および前記陰極エンドセルの第２のフランジ部の上部にも、該第２のフランジ部を貫通して設けられており、
前記陰極エンドセルに設けられた前記陽極液供給用流通部を通じて、前記電解槽の外部から陽極液が各陽極室に供給され、
前記陰極エンドセルに設けられた前記陰極液供給用流通部を通じて、前記電解槽の外部から陰極液が各陰極室に供給され、
前記陰極エンドセルに設けられた前記陽極液・ガス回収用流通部を通じて、陽極液および各陽極室中のガスが、各陽極室から前記電解槽の外部に取り出され、
前記陰極エンドセルに設けられた前記陰極液・ガス回収用流通部を通じて、陰極液および各陰極室中のガスが、各陰極室から前記電解槽の外部に取り出される、
請求項１～３のいずれかに記載の電解槽。 The catholyte supply flow section and the catholyte/gas recovery flow section are provided to penetrate the second flange of the cathode end cell,
The anolyte supply flow part is also provided at a lower part of the protective member of the second diaphragm element and a lower part of the second flange part of the cathode end cell, penetrating the second flange part,
The anolyte/gas recovery flow section is also provided above the protective member of the second diaphragm element and above the second flange section of the cathode end cell, penetrating the second flange section. Ori,
An anolyte is supplied to each anode chamber from outside the electrolytic cell through the anolyte supply flow section provided in the cathode end cell,
A catholyte is supplied to each cathode chamber from outside the electrolytic cell through the catholyte supply flow section provided in the cathode end cell,
The anolyte and the gas in each anode chamber are taken out from each anode chamber to the outside of the electrolytic cell through the anolyte/gas recovery flow section provided in the cathode end cell,
The catholyte and the gas in each cathode chamber are taken out from each cathode chamber to the outside of the electrolytic cell through the catholyte/gas recovery circulation section provided in the cathode end cell.
The electrolytic cell according to any one of claims 1 to 3.
請求項１～３のいずれかに記載の電解槽。 At least the surface of the protective member of each diaphragm element is formed of an electrically insulating resin material;
The electrolytic cell according to any one of claims 1 to 3.
前記陰極エンドセルに隣接して配置された、陰極側プレスフレームと、
をさらに備え、
前記積層構造が、前記陽極側プレスフレームと前記陰極側プレスフレームとの間に挟まれて締め付けられている、
請求項１～３のいずれかに記載の電解槽。 an anode side press frame disposed adjacent to the anode end cell;
a cathode side press frame disposed adjacent to the cathode end cell;
Furthermore,
The laminated structure is sandwiched and tightened between the anode side press frame and the cathode side press frame,
The electrolytic cell according to any one of claims 1 to 3.
（ａ）請求項１～３のいずれかに記載のアルカリ水電解用電解槽に、変動する直流電流を通電することにより、前記陰極液・ガス回収用流通部から水素ガスを回収する工程を含み、
前記工程（ａ）において、前記電解槽が前記変動する直流電流の最小値で運転されるときの単位時間あたりの主反応の水素ガス発生量が、前記電解槽が前記変動する直流電流の最大値で運転されるときの単位時間あたりの主反応の水素ガス発生量の１５％未満であることを特徴とする、ガス製造方法。 A method for producing at least hydrogen gas by electrolyzing alkaline water, the method comprising:
(a) a step of recovering hydrogen gas from the catholyte/gas recovery flow section by supplying a fluctuating direct current to the electrolytic cell for alkaline water electrolysis according to any one of claims 1 to 3; ,
In the step (a), when the electrolytic cell is operated at the minimum value of the fluctuating direct current, the amount of hydrogen gas generated in the main reaction per unit time is the maximum value of the fluctuating direct current. A method for producing gas, characterized in that the amount of hydrogen gas generated per unit time is less than 15% of the amount of hydrogen gas generated in the main reaction when operated at .
請求項１１に記載のガス製造方法。 The step (a) further includes recovering oxygen gas from the anolyte/gas recovery flow section,
The gas production method according to claim 11 .
請求項１１に記載のガス製造方法。 In the step (a), the pressure inside the anode chamber is maintained at +20 kPa or more with respect to atmospheric pressure.
The gas production method according to claim 11 .
請求項１１に記載のガス製造方法。 In the step (a), the pressure inside the cathode chamber is maintained at +20 kPa or more with respect to atmospheric pressure.
The gas production method according to claim 11 .
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