JP2021155818A5 - - Google Patents
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- JP2021155818A5 JP2021155818A5 JP2020058508A JP2020058508A JP2021155818A5 JP 2021155818 A5 JP2021155818 A5 JP 2021155818A5 JP 2020058508 A JP2020058508 A JP 2020058508A JP 2020058508 A JP2020058508 A JP 2020058508A JP 2021155818 A5 JP2021155818 A5 JP 2021155818A5
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- Prior art keywords
- electrode
- hydrogen peroxide
- water
- nickel salt
- nickel
- Prior art date
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- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims description 22
- 238000004519 manufacturing process Methods 0.000 claims description 9
- 150000002815 nickel Chemical class 0.000 claims description 6
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 5
- 238000000034 method Methods 0.000 claims description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 3
- 229910052799 carbon Inorganic materials 0.000 claims description 3
- 239000002131 composite material Substances 0.000 claims description 3
- 239000008151 electrolyte solution Substances 0.000 claims description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 2
- 229910052760 oxygen Inorganic materials 0.000 claims description 2
- 239000001301 oxygen Substances 0.000 claims description 2
- 239000000243 solution Substances 0.000 claims description 2
- 238000010298 pulverizing process Methods 0.000 claims 2
- 238000007654 immersion Methods 0.000 claims 1
- 239000002245 particle Substances 0.000 claims 1
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 4
- 239000003575 carbonaceous material Substances 0.000 description 4
- PYKYMHQGRFAEBM-UHFFFAOYSA-N anthraquinone Natural products CCC(=O)c1c(O)c2C(=O)C3C(C=CC=C3O)C(=O)c2cc1CC(=O)OC PYKYMHQGRFAEBM-UHFFFAOYSA-N 0.000 description 3
- 150000004056 anthraquinones Chemical class 0.000 description 3
- KBJMLQFLOWQJNF-UHFFFAOYSA-N nickel(ii) nitrate Chemical compound [Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O KBJMLQFLOWQJNF-UHFFFAOYSA-N 0.000 description 3
- 230000003647 oxidation Effects 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- 239000007772 electrode material Substances 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- 238000004659 sterilization and disinfection Methods 0.000 description 2
- 239000000758 substrate Substances 0.000 description 2
- RZVHIXYEVGDQDX-UHFFFAOYSA-N 9,10-anthraquinone Chemical compound C1=CC=C2C(=O)C3=CC=CC=C3C(=O)C2=C1 RZVHIXYEVGDQDX-UHFFFAOYSA-N 0.000 description 1
- 238000004061 bleaching Methods 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000003411 electrode reaction Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 230000000717 retained effect Effects 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 230000001954 sterilising effect Effects 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
Description
過酸化水素は、消毒、殺菌、漂白、洗浄、または酸化等に用いられており、工業的には２－アルキルアントラキノンの水素化と空気酸化を利用するアントラキノン法で製造されている（非特許文献１）。しかしながら、アントラキノン法は、アントラキノン誘導体および有機溶媒等の有機物を用いるため環境負荷が大きい。また、アントラキノン法による過酸化水素の製造は、分離操作等が必要となり高コストである。このため、他の工業的な過酸化水素の製造方法が検討されてきた。 Hydrogen peroxide is used for disinfection, sterilization, bleaching, cleaning, oxidation, etc., and is industrially produced by an anthraquinone method using hydrogenation of 2-alkylanthraquinone and air oxidation (non-patent literature 1). However, the anthraquinone method uses an anthraquinone derivative and an organic substance such as an organic solvent, which imposes a large burden on the environment. In addition, the production of hydrogen peroxide by the anthraquinone method requires a separation operation, etc., and is costly. Therefore, other industrial methods for producing hydrogen peroxide have been investigated.
さらに、炭酸塩を含む電解液を用いたアノード電極での水の酸化では、アノード電極として光電極を用いて光照射下で電極反応を行うことで、太陽光等の光エネルギーが利用できる。このため、外部電圧を印加せず、または低く抑えた外部電圧を印加して、低コストで過酸化水素を製造する方法も提案されている（非特許文献３および特許文献６）。また、酸化処理した導電性炭素材料を電極材料として用いたカソード電極と、光電極を用いたアノード電極を組み合わせることにより、カソード電極における酸素の還元と、炭酸塩を含む電解液を用いたアノード電極における光照射下で水の酸化を同時に行って、高い電流効率で効率的に、過酸化水素を両極で製造する方法が提案されている（特許文献７）。 Furthermore, in the oxidation of water at an anode electrode using an electrolytic solution containing a carbonate, light energy such as sunlight can be used by using a photoelectrode as the anode electrode and performing an electrode reaction under light irradiation. Therefore, a method for producing hydrogen peroxide at low cost without applying an external voltage or applying a low external voltage has been proposed ( Non-Patent Document 3 and Patent Document 6). Further, by combining a cathode electrode using an oxidized conductive carbon material as an electrode material and an anode electrode using a photoelectrode, reduction of oxygen in the cathode electrode and anode electrode using an electrolytic solution containing a carbonate can be achieved. A method has been proposed in which water is simultaneously oxidized under light irradiation in , and hydrogen peroxide is efficiently produced at both electrodes with high current efficiency (Patent Document 7).
本願発明者らは、従来技術を検討し、カソード電極のさらなる性能向上を目指して様々な条件で実験を進めた。その結果、カソード電極の材料として用いられていた導電性炭素材料に新たにニッケル塩を添加することで、過酸化水素の製造における性能が向上することを見出した。また、本願のニッケル塩を含有する導電性炭素材料は、炭酸塩を含む液体に浸漬することにより性能が向上することを見出した。 The inventors of the present application have studied conventional techniques and conducted experiments under various conditions with the aim of further improving the performance of the cathode electrode. As a result, it was found that the addition of a nickel salt to the conductive carbon material used as the cathode electrode material improved the performance in the production of hydrogen peroxide. Moreover, it was found that the performance of the conductive carbon material containing the nickel salt of the present application is improved by immersing it in a liquid containing a carbonate.
（実施例２～実施例４）
表１に示す硝酸ニッケルの含有量を変更した点を除き、実施例１と同様にして実施例２～実施例４のカソード電極を作製した。カーボンペーパー基材上のニッケルの保持量をＸＲＦから見積もった。その結果、実施例２では２．６μｇ／ｃｍ２、実施例４では２４．５μｇ／ｃｍ２であった。硝酸ニッケルの含有量におおむね比例してカーボンペーパー基材上にニッケル塩が保持されていた。また、実施例１と同様にして、実施例２～実施例４のカソード電極を用いて過酸化水素を製造した。過酸化水素生成時の電流効率と電流密度を表１に示す。
(Examples 2 to 4)
Cathode electrodes of Examples 2 to 4 were produced in the same manner as in Example 1, except that the content of nickel nitrate shown in Table 1 was changed. The nickel retention on the carbon paper substrate was estimated from XRF. As a result, it was 2.6 μg/cm 2 in Example 2 and 24.5 μg/cm 2 in Example 4. The nickel salt was retained on the carbon paper substrate roughly proportional to the nickel nitrate content. Further, in the same manner as in Example 1, using the cathode electrodes of Examples 2 to 4, hydrogen peroxide was produced. Table 1 shows the current efficiency and current density during hydrogen peroxide production.
（実施例５～実施例１０）
表２に示すニッケル塩を用いた点を除き、実施例２と同様にして実施例５～実施例１０のカソード電極を作製した。また、実施例１と同様にして、実施例５～実施例１０のカソード電極を用いて過酸化水素を製造した。過酸化水素生成時の電流効率と電流密度を表２に示す。
(Examples 5 to 10)
Cathode electrodes of Examples 5 to 10 were produced in the same manner as in Example 2, except that the nickel salts shown in Table 2 were used. Further, in the same manner as in Example 1 , using the cathode electrodes of Examples 5 to 10, hydrogen peroxide was produced. Table 2 shows the current efficiency and current density during hydrogen peroxide production.
表２の実施例１１に示すように、導電性炭素材料と水溶性の硝酸ニッケルを含有する複合体を、炭酸イオンを含む溶液に浸漬することにより、その後に水で洗浄してもニッケル成分が複合体からあまり除去されず、電流効率８２％、電流密度７．９ｍＡ／ｃｍ２となり、実施例２と同様に好ましい結果が得られた。また、実施例１２では、８３％の高い電流効率に加え、１２．０ｍＡ／ｃｍ２の大きな電流密度が得られた。 As shown in Example 11 in Table 2, by immersing a composite containing a conductive carbon material and water-soluble nickel nitrate in a solution containing carbonate ions, the nickel component was removed even after washing with water. Not much was removed from the composite, and the current efficiency was 82% and the current density was 7.9 mA/cm 2 . In Example 12, a high current density of 12.0 mA/cm 2 was obtained in addition to a high current efficiency of 83%.
Claims (2)
前記ニッケル塩が水溶性であり、
前記混合粉砕工程では、前記導電性炭素粒子と前記ニッケル塩を水中で混合し、
前記混合粉砕工程の後、前記複合体を炭酸塩の水溶液に浸漬する浸漬工程をさらに有する電極の製造方法。 In claim 8 or 9,
the nickel salt is water-soluble,
In the mixing pulverization step, the conductive carbon particles and the nickel salt are mixed in water,
A method for manufacturing an electrode, further comprising an immersion step of immersing the composite in an aqueous carbonate solution after the mixing and pulverizing step.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2020058508A JP7466182B2 (en) | 2020-03-27 | 2020-03-27 | Electrode and method for producing hydrogen peroxide using said electrode |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2020058508A JP7466182B2 (en) | 2020-03-27 | 2020-03-27 | Electrode and method for producing hydrogen peroxide using said electrode |
Publications (3)
| Publication Number | Publication Date |
|---|---|
| JP2021155818A JP2021155818A (en) | 2021-10-07 |
| JP2021155818A5 true JP2021155818A5 (en) | 2023-01-30 |
| JP7466182B2 JP7466182B2 (en) | 2024-04-12 |
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| Application Number | Title | Priority Date | Filing Date |
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| JP2020058508A Active JP7466182B2 (en) | 2020-03-27 | 2020-03-27 | Electrode and method for producing hydrogen peroxide using said electrode |
Country Status (1)
| Country | Link |
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| JP (1) | JP7466182B2 (en) |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114249391A (en) * | 2021-12-15 | 2022-03-29 | 盐城工学院 | Preparation method of activated carbon column loaded nickel phosphate particle electrode |
Family Cites Families (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP4368166B2 (en) | 2003-08-28 | 2009-11-18 | 旭化成ケミカルズ株式会社 | Fuel cell reactor |
| JP4919941B2 (en) | 2006-12-28 | 2012-04-18 | トヨタ自動車株式会社 | Inspection method for polymer electrolyte membrane |
| JP2009068080A (en) | 2007-09-14 | 2009-04-02 | Tokyo Institute Of Technology | Fuel cell type reaction apparatus and method of manufacturing compound using the same |
| JP5510181B2 (en) | 2010-08-18 | 2014-06-04 | 凸版印刷株式会社 | Electrocatalyst layer production method and polymer electrolyte fuel cell |
| JP2019157223A (en) | 2018-03-14 | 2019-09-19 | 国立研究開発法人産業技術総合研究所 | Production method of hydrogen peroxide using photoelectrode |
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