JP2012011297A5 - - Google Patents
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- JP2012011297A5 JP2012011297A5 JP2010149334A JP2010149334A JP2012011297A5 JP 2012011297 A5 JP2012011297 A5 JP 2012011297A5 JP 2010149334 A JP2010149334 A JP 2010149334A JP 2010149334 A JP2010149334 A JP 2010149334A JP 2012011297 A5 JP2012011297 A5 JP 2012011297A5
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- 239000000463 material Substances 0.000 description 42
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 10
- 239000002243 precursor Substances 0.000 description 8
- 239000003575 carbonaceous material Substances 0.000 description 7
- 238000001027 hydrothermal synthesis Methods 0.000 description 7
- 229910052751 metal Inorganic materials 0.000 description 7
- 239000000203 mixture Substances 0.000 description 7
- 239000002002 slurry Substances 0.000 description 7
- 239000007788 liquid Substances 0.000 description 6
- 238000002156 mixing Methods 0.000 description 5
- 239000002994 raw material Substances 0.000 description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 239000004020 conductor Substances 0.000 description 4
- 239000010411 electrocatalyst Substances 0.000 description 4
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 3
- 238000001354 calcination Methods 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 3
- 125000004435 hydrogen atom Chemical class [H]* 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 150000002736 metal compounds Chemical class 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 229910052796 boron Inorganic materials 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 229910052801 chlorine Inorganic materials 0.000 description 2
- 239000000460 chlorine Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- -1 nitrogen-containing compound Chemical class 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 239000011593 sulfur Substances 0.000 description 2
- 125000004432 carbon atom Chemical group C* 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 239000012018 catalyst precursor Substances 0.000 description 1
- 125000001309 chloro group Chemical group Cl* 0.000 description 1
- 238000007580 dry-mixing Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 125000004433 nitrogen atom Chemical group N* 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 125000004434 sulfur atom Chemical group 0.000 description 1
Description
すなわち本発明は、下記の手段を提供する。
＜１＞以下の第一材料、以下の第二材料および以下の第三材料を含有する混合物を、超臨界状態または亜臨界状態の水の存在下において水熱反応させて得られる電極触媒の前駆体を、以下の第二材料が炭素材料に変化する条件にて焼成する工程を含む電極触媒の製造方法：
第一材料は、４Ａ族元素および５Ａ族元素からなる群より選択される１種以上の金属元素と、水素、窒素、塩素、炭素、硼素、硫黄および酸素からなる群より選択される１種以上の非金属元素とで構成される金属化合物であり、
第二材料は、炭素材料前駆体であり、
第三材料は、導電性材料である。
＜２＞以下の第一材料、以下の第二材料、以下の第三材料および以下の第四材料を含有する混合物を、超臨界状態または亜臨界状態の水の存在下において水熱反応させて得られる電極触媒の前駆体を、第二材料が炭素材料に変化する条件にて焼成する工程を含む電極触媒の製造方法：
第一材料は、４Ａ族元素および５Ａ族元素からなる群より選択される１種以上の金属元素と、水素原子、窒素原子、塩素原子、炭素原子、硼素原子、硫黄原子および酸素原子からなる群より選択される１種以上の非金属元素とで構成される金属化合物であり
第二材料は、炭素材料前駆体であり、
第三材料は、導電性材料であり、
第四材料は、窒素含有化合物である。
＜３＞第一材料における前記金属元素が、ＺｒまたはＴｉである＜１＞または<２>に記載の方法。
＜４＞第三材料における前記導電性材料が、カーボンブラックである＜１＞〜＜３＞のいずれかに記載の方法。
＜５＞前記焼成の雰囲気が、無酸素の雰囲気である＜１＞〜＜４＞のいずれかに記載の方法。
That is, the present invention provides the following means.
<1> Electrocatalyst precursor obtained by hydrothermal reaction of a mixture containing the following first material, the following second material, and the following third material in the presence of supercritical or subcritical water A method for producing an electrocatalyst comprising a step of calcining a body under conditions where the following second material is changed to a carbon material:
The first material is one or more metal elements selected from the group consisting of Group 4A elements and Group 5A elements, and one or more selected from the group consisting of hydrogen, nitrogen, chlorine, carbon, boron, sulfur and oxygen A non-metallic element composed of a metal compound,
The second material is a carbon material precursor,
The third material is a conductive material.
<2> Hydrothermal reaction of a mixture containing the following first material, the following second material, the following third material, and the following fourth material in the presence of supercritical or subcritical water. A method for producing an electrode catalyst, comprising a step of calcining the obtained electrode catalyst precursor under a condition that the second material is changed to a carbon material :
The first material is a group consisting of one or more metal elements selected from the group consisting of Group 4A elements and Group 5A elements, and hydrogen atoms, nitrogen atoms, chlorine atoms, carbon atoms, boron atoms, sulfur atoms and oxygen atoms. A metal compound composed of one or more non-metallic elements selected from the second material is a carbon material precursor;
The third material is a conductive material,
The fourth material is a nitrogen-containing compound.
<3> The method according to <1> or <2>, wherein the metal element in the first material is Zr or Ti.
<4> The method according to any one of <1> to <3>, wherein the conductive material in the third material is carbon black.
<5> The method according to any one of <1> to <4>, wherein the firing atmosphere is an oxygen-free atmosphere.
（第二の発明）
本発明の電極触媒の製造方法は、以下の第一材料、以下の第二材料、以下の第三材料および以下の第四材料を含有する混合物を、超臨界状態または亜臨界状態の水の存在下において水熱反応させて得られる電極触媒の前駆体を、第二材料が炭素材料に変化する条件にて焼成する工程を含む。
第一材料は、４Ａ族元素および５Ａ族元素からなる群より選択される１種以上の金属元素と、水素、窒素、塩素、炭素、硼素、硫黄および酸素からなる群より選択される１種以上の非金属元素とで構成される金属化合物であり
第二材料は、炭素材料前駆体であり、
第三材料は、導電性材料であり、
第四材料は、窒素含有化合物である。
(Second invention)
The method for producing an electrocatalyst according to the present invention comprises a mixture containing the following first material, the following second material, the following third material, and the following fourth material, the presence of water in a supercritical state or a subcritical state. A step of calcining a precursor of an electrode catalyst obtained by hydrothermal reaction under a condition that the second material is changed to a carbon material.
The first material is one or more metal elements selected from the group consisting of Group 4A elements and Group 5A elements, and one or more selected from the group consisting of hydrogen, nitrogen, chlorine, carbon, boron, sulfur and oxygen The second material is a carbon material precursor, which is a metal compound composed of a non-metallic element of
The third material is a conductive material,
The fourth material is a nitrogen-containing compound.
上記第一の発明においては、上記第一材料、上記第二材料および上記第三材料を含有する混合物を、超臨界状態または亜臨界状態の水の存在下において水熱反応させて電極触媒の前駆体を得る。また、上記の第二の発明においては、上記第一材料、上記第二材料、上記第三材料および上記第四材料を含有する混合物を、超臨界状態または亜臨界状態の水の存在下において水熱反応させて電極触媒の前駆体を得る。上記混合には、ボールミル、Ｖ型混合機、攪拌機等の、工業的に通常用いられている装置を用いることができる。このときの混合は、乾式混合、湿式混合のいずれによってもよい。また、湿式混合の後には、炭素材料前駆体が分解しない程度の温度で乾燥を行ってもよい。
In the first invention, a mixture containing the first material, the second material, and the third material is subjected to a hydrothermal reaction in the presence of water in a supercritical state or a subcritical state to produce a precursor of an electrode catalyst. Get the body. In the second invention, the mixture containing the first material, the second material, the third material, and the fourth material is mixed with water in the presence of water in a supercritical state or a subcritical state. The precursor of the electrocatalyst is obtained by heat reaction. For the above-described mixing, industrially used apparatuses such as a ball mill, a V-type mixer, and a stirrer can be used. The mixing at this time may be either dry mixing or wet mixing. In addition, after the wet mixing, drying may be performed at a temperature at which the carbon material precursor is not decomposed.
以下に、本発明において連続的に水熱反応を行うための反応装置について、図面を参照しながら説明する。図１は、連続的に水熱反応を行うための流通式反応装置の概要を示す図である。水タンク１１，２１は、水を供給するためのタンクである。原料タンク２２は、原料スラリーを供給するためのタンクである。弁１１０，２１０，２２０を開けることにより、これらのタンクから液が供給される。上記の第一の発明の場合、上記原料スラリーは第一材料、第二材料および第三材料を含む混合物のスラリーまたは水溶液であり、また、上記の第二の発明の場合、上記原料スラリーは第一材料、第二材料、第三材料および第四材料を含む混合物のスラリーまたは水溶液である。送液ポンプ１３の駆動により水タンク１１から加熱器１４に液が送られ、送液ポンプ２３の駆動により水タンク２１または原料タンク２２から加熱器２４に液が送られる。送られたそれぞれの液は、混合部３０で混合され、主に反応器４０内で水熱反応する。図２は、反応器の概要を示す図である。反応器４０内には、内部配管４１とその配管を加熱する加熱器４４があり、内部配管４１は外部の配管に接続されている。水熱反応後、生成したスラリーは、冷却器５１により冷却され、背圧弁５３を通過して、回収容器６０で回収される。
Below, the reaction apparatus for performing a hydrothermal reaction continuously in this invention is demonstrated, referring drawings. FIG. 1 is a diagram showing an outline of a flow reactor for continuously performing a hydrothermal reaction. The water tanks 11 and 21 are tanks for supplying water. The raw material tank 22 is a tank for supplying the raw material slurry. By opening the valves 110, 210, and 220, liquid is supplied from these tanks. In the case of the first invention, the raw material slurry is a slurry or an aqueous solution of a mixture containing the first material , the second material and the third material , and in the case of the second invention, the raw material slurry is the first material slurry. A slurry or aqueous solution of a mixture comprising one material , a second material, a third material and a fourth material . The liquid is sent from the water tank 11 to the heater 14 by driving the liquid feed pump 13, and the liquid is sent from the water tank 21 or the raw material tank 22 to the heater 24 by driving the liquid feed pump 23. The sent liquids are mixed in the mixing unit 30 and mainly hydrothermally react in the reactor 40. FIG. 2 is a diagram showing an outline of the reactor. In the reactor 40, there is an internal pipe 41 and a heater 44 for heating the pipe, and the internal pipe 41 is connected to an external pipe. After the hydrothermal reaction, the generated slurry is cooled by the cooler 51, passes through the back pressure valve 53, and is collected in the collection container 60.
Priority Applications (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2010149334A JP2012011297A (en) | 2010-06-30 | 2010-06-30 | Method for producing electrode catalyst |
| PCT/JP2011/065235 WO2012002550A1 (en) | 2010-06-30 | 2011-06-27 | Method for producing electrode catalyst |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2010149334A JP2012011297A (en) | 2010-06-30 | 2010-06-30 | Method for producing electrode catalyst |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JP2012011297A JP2012011297A (en) | 2012-01-19 |
| JP2012011297A5 true JP2012011297A5 (en) | 2013-06-06 |
Family
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Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP2010149334A Withdrawn JP2012011297A (en) | 2010-06-30 | 2010-06-30 | Method for producing electrode catalyst |
Country Status (2)
| Country | Link |
|---|---|
| JP (1) | JP2012011297A (en) |
| WO (1) | WO2012002550A1 (en) |
Families Citing this family (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TWI481106B (en) * | 2013-09-26 | 2015-04-11 | Univ Nat Taiwan Science Tech | Preparing method of catalyst for fuel cell and preparing method of membrane electrode assembly |
| CN112517061B (en) * | 2020-12-03 | 2022-05-20 | 北方民族大学 | Sulfonic acid type solid acid catalyst and preparation method thereof |
| CN113224331B (en) * | 2021-05-08 | 2022-05-13 | 中北大学 | Alkaline system direct urea fuel cell anode catalyst and preparation method thereof |
Family Cites Families (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009082910A (en) * | 2007-09-14 | 2009-04-23 | Toyota Motor Corp | Fine-particle composite, process for producing the fine-particle composite, catalyst for solid polymer electrolyte fuel cell, and solid polymer electrolyte fuel cell |
| JP5353287B2 (en) * | 2008-03-21 | 2013-11-27 | 住友化学株式会社 | Electrocatalyst production method and electrode catalyst |
| JP2009298601A (en) * | 2008-06-10 | 2009-12-24 | Sumitomo Chemical Co Ltd | Method for producing metal oxynitride |
| JP5146121B2 (en) * | 2008-06-10 | 2013-02-20 | 住友化学株式会社 | Method for producing metal carbonitride |
| JP2010227843A (en) * | 2009-03-27 | 2010-10-14 | Sumitomo Chemical Co Ltd | Method for producing electrode catalyst, and electrode catalyst |
| KR20120100707A (en) * | 2009-06-26 | 2012-09-12 | 스미또모 가가꾸 가부시끼가이샤 | Method for producing electrode catalyst |
-
2010
- 2010-06-30 JP JP2010149334A patent/JP2012011297A/en not_active Withdrawn
-
2011
- 2011-06-27 WO PCT/JP2011/065235 patent/WO2012002550A1/en active Application Filing
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