JPH04329888A - Electrode consisting of titanium boride and high-potential electrolysis utilizing this electrode - Google Patents
Electrode consisting of titanium boride and high-potential electrolysis utilizing this electrodeInfo
- Publication number
- JPH04329888A JPH04329888A JP3099986A JP9998691A JPH04329888A JP H04329888 A JPH04329888 A JP H04329888A JP 3099986 A JP3099986 A JP 3099986A JP 9998691 A JP9998691 A JP 9998691A JP H04329888 A JPH04329888 A JP H04329888A
- Authority
- JP
- Japan
- Prior art keywords
- electrode
- titanium boride
- materials
- carbon dioxide
- reductional
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 title claims abstract description 16
- 239000010936 titanium Substances 0.000 title claims abstract description 16
- 229910052719 titanium Inorganic materials 0.000 title claims abstract description 16
- 238000005868 electrolysis reaction Methods 0.000 title claims description 12
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims abstract description 30
- 239000001569 carbon dioxide Substances 0.000 claims abstract description 15
- 229910002092 carbon dioxide Inorganic materials 0.000 claims abstract description 15
- 239000000126 substance Substances 0.000 claims description 7
- 239000007864 aqueous solution Substances 0.000 claims description 5
- 238000000034 method Methods 0.000 claims description 5
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 abstract description 6
- 239000000463 material Substances 0.000 abstract description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 2
- DMLAVOWQYNRWNQ-UHFFFAOYSA-N azobenzene Chemical compound C1=CC=CC=C1N=NC1=CC=CC=C1 DMLAVOWQYNRWNQ-UHFFFAOYSA-N 0.000 abstract description 2
- 239000010953 base metal Substances 0.000 abstract description 2
- 239000011230 binding agent Substances 0.000 abstract description 2
- 229910021645 metal ion Inorganic materials 0.000 abstract description 2
- 239000001301 oxygen Substances 0.000 abstract description 2
- 229910052760 oxygen Inorganic materials 0.000 abstract description 2
- 239000002245 particle Substances 0.000 abstract description 2
- 238000005245 sintering Methods 0.000 abstract description 2
- 238000004898 kneading Methods 0.000 abstract 1
- 238000000465 moulding Methods 0.000 abstract 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 7
- 239000001257 hydrogen Substances 0.000 description 7
- 229910052739 hydrogen Inorganic materials 0.000 description 7
- 238000006722 reduction reaction Methods 0.000 description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 239000003054 catalyst Substances 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- 230000002829 reductive effect Effects 0.000 description 4
- 238000000354 decomposition reaction Methods 0.000 description 3
- 239000002574 poison Substances 0.000 description 3
- 231100000614 poison Toxicity 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- AZQWKYJCGOJGHM-UHFFFAOYSA-N 1,4-benzoquinone Chemical compound O=C1C=CC(=O)C=C1 AZQWKYJCGOJGHM-UHFFFAOYSA-N 0.000 description 2
- QYEXBYZXHDUPRC-UHFFFAOYSA-N B#[Ti]#B Chemical compound B#[Ti]#B QYEXBYZXHDUPRC-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 238000002484 cyclic voltammetry Methods 0.000 description 2
- 239000007791 liquid phase Substances 0.000 description 2
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 2
- 229910052753 mercury Inorganic materials 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- LQNUZADURLCDLV-UHFFFAOYSA-N nitrobenzene Chemical compound [O-][N+](=O)C1=CC=CC=C1 LQNUZADURLCDLV-UHFFFAOYSA-N 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- 239000002243 precursor Substances 0.000 description 2
- 238000001644 13C nuclear magnetic resonance spectroscopy Methods 0.000 description 1
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 1
- 229910033181 TiB2 Inorganic materials 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- RWCCWEUUXYIKHB-UHFFFAOYSA-N benzophenone Chemical compound C=1C=CC=CC=1C(=O)C1=CC=CC=C1 RWCCWEUUXYIKHB-UHFFFAOYSA-N 0.000 description 1
- 239000012965 benzophenone Substances 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- 238000001460 carbon-13 nuclear magnetic resonance spectrum Methods 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000005518 electrochemistry Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 235000019253 formic acid Nutrition 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- BAZAXWOYCMUHIX-UHFFFAOYSA-M sodium perchlorate Chemical compound [Na+].[O-]Cl(=O)(=O)=O BAZAXWOYCMUHIX-UHFFFAOYSA-M 0.000 description 1
- 229910001488 sodium perchlorate Inorganic materials 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 239000011135 tin Substances 0.000 description 1
Abstract
Description
【０００１】0001
【産業上の利用分野】本発明は、硼化チタンからなる電
極及びこれを利用した水溶液中の還元性電気分解に係わ
り、特に高電位を要する難還元性の物質を、特別な触媒
毒を用いる事なく電気分解する方法に関する。[Industrial Application Field] The present invention relates to an electrode made of titanium boride and reductive electrolysis in an aqueous solution using the same. Concerning how to perform electrolysis without any problems.
【０００２】0002
【従来の技術】従来、水溶液中の高電位電気分解還元反
応の電極、特に陰極としては水銀が多く用いられてきた
。最近、より困難な反応として二酸化炭素の電気分解還
元反応が注目されているが、この目的のため、水銀も含
め３０種近くの金属元素の電極について電気分解還元反
応の研究がおこなわれ、例えば銅電極がこの目的に適す
る等の報告がある（伊藤 要、「電気化学および工業
物理化学」、第５８巻、第１１号、９４８頁及び堀
善夫、 同上、９９６頁）。BACKGROUND OF THE INVENTION Conventionally, mercury has been widely used as an electrode, particularly a cathode, for high-potential electrolytic reduction reactions in aqueous solutions. Recently, the electrolytic reduction reaction of carbon dioxide has been attracting attention as a more difficult reaction.For this purpose, research has been conducted on the electrolytic reduction reaction using electrodes made of nearly 30 metal elements, including mercury. There are reports that electrodes are suitable for this purpose (Kaname Ito, "Electrochemistry and Industrial Physical Chemistry", Vol. 58, No. 11, p. 948 and Hori
Yoshio, ibid., p. 996).
【０００３】金属電極は比較的低い水素過電圧を持ち、
二酸化炭素の存在しない系では、二酸化炭素の分解電圧
よりはるかに低い電極電圧で、水を分解して水素を発生
せしめる。二酸化炭素が存在する場合には、なんらかの
機構（おそらく電気分解還元により生成した一酸化炭素
の電極面への吸着）により、水素発生に対する触媒毒が
生成し、水素発生が妨げられてより高電位の電気分解反
応が可能になる。しかし、触媒毒またはその先駆体を特
別に添加しなくても、高電位の電気分解還元反応を可能
ならしめる電極があれば、極めて有益である。Metal electrodes have relatively low hydrogen overpotentials;
In a system without carbon dioxide, water is decomposed to generate hydrogen at an electrode voltage that is much lower than the decomposition voltage of carbon dioxide. In the presence of carbon dioxide, some mechanism (probably adsorption of carbon monoxide produced by electrolytic reduction to the electrode surface) forms a catalyst poison for hydrogen evolution, preventing hydrogen evolution and forcing it to reach higher potentials. Electrolytic reactions become possible. However, it would be extremely beneficial to have an electrode that allows high potential electrolytic reduction reactions without the specific addition of catalyst poisons or their precursors.
【０００４】0004
【発明が解決しようとする課題】従って本発明の目的は
、高い水素過電圧を有し、触媒毒またはその先駆体を特
別に添加しなくても、高電位の電気分解還元反応を可能
ならしめる電極、並びにそれを使用して難還元性物質を
電気分解還元する方法を提供することである。SUMMARY OF THE INVENTION Therefore, it is an object of the present invention to provide an electrode which has a high hydrogen overvoltage and which enables a high potential electrolytic reduction reaction without the special addition of a catalyst poison or its precursor. , and a method of electrolytically reducing a refractory substance using the same.
【０００５】[0005]
【課題を解決するための手段】本発明者は上記目的を達
成するために種々検討した結果、高硬度材料として知ら
れている硼化チタンが例外的に高い水素過電圧を持つ事
を発見した。本発明はこの発見に基づいてなされたもの
である。すなわち本発明は、硼化チタンからなる電極を
提供するものである。この電極は、高電位電気分解用の
電極として有用であり、特に高電位電気分解用の陰極と
して有用である。[Means for Solving the Problems] As a result of various studies to achieve the above object, the present inventor discovered that titanium boride, which is known as a highly hard material, has an exceptionally high hydrogen overvoltage. The present invention has been made based on this discovery. That is, the present invention provides an electrode made of titanium boride. This electrode is useful as an electrode for high potential electrolysis, and particularly useful as a cathode for high potential electrolysis.
【０００６】本発明はさらに、硼化チタンからなる電極
を陰極として使用し、水溶液中の難還元性物質を電気分
解することを特徴とする難還元性物質の還元方法を提供
するものである。この際、陰極電圧としては、＋０．５
〜−３．０Ｖが適当である。本発明方法が適用される難
還元性物質としては、二酸化炭素、酸素、卑金属イオン
（例えば、ニッケル、コバルト、スズ、カドミウム等）
、各種有機化合物（例えば、アゾベンゼン、ベンゾフェ
ノン、キノン、ニトロベンゼン等）等が挙げられる。The present invention further provides a method for reducing a refractory substance, which comprises electrolyzing the refractory substance in an aqueous solution using an electrode made of titanium boride as a cathode. At this time, the cathode voltage is +0.5
~-3.0V is appropriate. Examples of refractory substances to which the method of the present invention is applied include carbon dioxide, oxygen, and base metal ions (e.g., nickel, cobalt, tin, cadmium, etc.)
, various organic compounds (for example, azobenzene, benzophenone, quinone, nitrobenzene, etc.).
【０００７】本発明の硼化チタン電極は、硼化チタン粒
子に適当なバインダーを適当量混合し、適当な形状に成
形後、焼結することにより容易に作製することができる
。また、市販されている硼化チタン焼結体（日本鋼管製
ＴｉＢ２焼結体）も有利に使用することができる。The titanium boride electrode of the present invention can be easily produced by mixing titanium boride particles with an appropriate amount of a suitable binder, shaping the mixture into a suitable shape, and then sintering the mixture. In addition, a commercially available titanium boride sintered body (TiB2 sintered body manufactured by Nippon Kokan Co., Ltd.) can also be advantageously used.
【０００８】[0008]
【発明の効果】本発明の電極を用いることにより、非常
に簡単に高電位の還元性電気分解が可能になる。電極自
身が高い水素過電圧を持っているため、これを特定の反
応、例えば二酸化炭素のメタノールへの変換、のための
触媒などと組み合わせる場合の自由度が、非常に大きい
。また、本発明の電極は、通常の電気分解条件下で極め
て安定であり、毒性もないので環境破壊や公害発生等の
問題がない。[Effects of the Invention] By using the electrode of the present invention, high-potential reductive electrolysis becomes possible very easily. The high hydrogen overpotential of the electrode itself provides great flexibility in combining it with catalysts for specific reactions, such as the conversion of carbon dioxide to methanol. Further, the electrode of the present invention is extremely stable under normal electrolysis conditions and is non-toxic, so there are no problems such as environmental destruction or pollution.
【０００９】[0009]
【実施例】硼化チタンを陰極、銀を参照電極として１Ｍ
過塩素酸ナトリウムの水溶液に漬け、その電流・電圧特
性をサイクリック・ボルタンメトリー法で測定した。ま
ず、窒素を流した場合の電流値を測定し、次いで二酸化
炭素を加えて流した場合の電流値を測定した。それぞれ
の電位で、二酸化炭素を加えて流した場合の電流値から
窒素を流した場合の電流値を差し引き、電位と差し引い
た電流値をプロットしたのが図１である。この図から明
らかなように、−０．７Ｖ付近から電流値の増加が見ら
れ、−１．０Ｖ付近で定常値に達する。これらの事実は
、二酸化炭素が還元されたことを示すものである。これ
に対して従来の電極、例えば、プラチナ電極では−０．
６Ｖ付近から、水の分解による電流値の急峻な増加が見
られる。このことは、本発明の硼化チタン電極では、−
１．５Ｖ程度まで水の分解が事実上起こらないことを示
している。[Example] 1M using titanium boride as a cathode and silver as a reference electrode
It was immersed in an aqueous solution of sodium perchlorate, and its current and voltage characteristics were measured using cyclic voltammetry. First, the current value when nitrogen was flowed was measured, and then the current value when carbon dioxide was added and flowed was measured. At each potential, the current value when nitrogen is flowed is subtracted from the current value when carbon dioxide is added and flowed, and the potential and the subtracted current value are plotted in FIG. As is clear from this figure, the current value increases from around -0.7V and reaches a steady value around -1.0V. These facts indicate that carbon dioxide has been reduced. In contrast, conventional electrodes, for example platinum electrodes, have a -0.
A sharp increase in current value due to water decomposition can be seen from around 6V. This means that in the titanium boride electrode of the present invention, -
This shows that virtually no water decomposition occurs up to about 1.5V.
【００１０】次に二酸化炭素還元生成物について調べた
。電気分解後の気相を検知管により分析し、一酸化炭素
が生成していることを確認した。また、電気分解後の液
相を１３Ｃ−ＮＭＲで分析し、ギ酸が生成していること
を確認した。結果を図２に示す。これらの事実は、二酸
化炭素が還元されたことを明確に示すものである。Next, carbon dioxide reduction products were investigated. The gas phase after electrolysis was analyzed using a detection tube, and it was confirmed that carbon monoxide was produced. Furthermore, the liquid phase after electrolysis was analyzed by 13C-NMR, and it was confirmed that formic acid was produced. The results are shown in Figure 2. These facts clearly indicate that carbon dioxide has been reduced.
【図１】実施例の電気分解セルを用いて、二酸化炭素を
流した場合の電流・電圧特性をサイクリック・ボルタン
メトリー法で測定した結果を示す図面である。FIG. 1 is a drawing showing the results of measuring current and voltage characteristics by cyclic voltammetry when carbon dioxide is passed through an electrolytic cell according to an example.
【図２】実施例の電気分解後の液相の１３Ｃ−ＮＭＲス
ペクトルを示す図面である。FIG. 2 is a diagram showing a 13C-NMR spectrum of a liquid phase after electrolysis in an example.
Claims (5)
。2. A high potential electrolysis electrode made of titanium boride.
。3. A cathode for high potential electrolysis made of titanium boride.
し、水溶液中の難還元性物質を電気分解することを特徴
とする難還元性物質の還元方法。4. A method for reducing a refractory substance, which comprises electrolyzing a refractory substance in an aqueous solution using an electrode made of titanium boride as a cathode.
記載の方法。Claim 5: Claim 4 wherein the refractory substance is carbon dioxide.
Method described.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3099986A JPH04329888A (en) | 1991-05-01 | 1991-05-01 | Electrode consisting of titanium boride and high-potential electrolysis utilizing this electrode |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3099986A JPH04329888A (en) | 1991-05-01 | 1991-05-01 | Electrode consisting of titanium boride and high-potential electrolysis utilizing this electrode |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH04329888A true JPH04329888A (en) | 1992-11-18 |
Family
ID=14261979
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP3099986A Pending JPH04329888A (en) | 1991-05-01 | 1991-05-01 | Electrode consisting of titanium boride and high-potential electrolysis utilizing this electrode |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH04329888A (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2011135781A1 (en) * | 2010-04-26 | 2011-11-03 | パナソニック株式会社 | Method for reducing carbon dioxide |
| WO2012011209A1 (en) * | 2010-07-23 | 2012-01-26 | パナソニック株式会社 | Method for reducing carbon dioxide |
| US8597488B2 (en) | 2010-04-26 | 2013-12-03 | Panasonic Corporation | Method for reducing carbon dioxide |
-
1991
- 1991-05-01 JP JP3099986A patent/JPH04329888A/en active Pending
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2011135781A1 (en) * | 2010-04-26 | 2011-11-03 | パナソニック株式会社 | Method for reducing carbon dioxide |
| US8597488B2 (en) | 2010-04-26 | 2013-12-03 | Panasonic Corporation | Method for reducing carbon dioxide |
| WO2012011209A1 (en) * | 2010-07-23 | 2012-01-26 | パナソニック株式会社 | Method for reducing carbon dioxide |
| JP4907748B2 (en) * | 2010-07-23 | 2012-04-04 | パナソニック株式会社 | How to reduce carbon dioxide |
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