JPH04156947A - Combustion catalyst - Google Patents
Combustion catalystInfo
- Publication number
- JPH04156947A JPH04156947A JP27938990A JP27938990A JPH04156947A JP H04156947 A JPH04156947 A JP H04156947A JP 27938990 A JP27938990 A JP 27938990A JP 27938990 A JP27938990 A JP 27938990A JP H04156947 A JPH04156947 A JP H04156947A
- Authority
- JP
- Japan
- Prior art keywords
- base material
- supported
- combustion catalyst
- catalyst
- silicon carbide
- 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.)
- Granted
Links
- 239000003054 catalyst Substances 0.000 title claims abstract description 29
- 238000002485 combustion reaction Methods 0.000 title claims abstract description 24
- 239000000463 material Substances 0.000 claims abstract description 23
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims abstract description 12
- 229910010271 silicon carbide Inorganic materials 0.000 claims abstract description 10
- 229910052763 palladium Inorganic materials 0.000 claims abstract description 7
- 239000011301 petroleum pitch Substances 0.000 claims abstract description 7
- 229910052697 platinum Inorganic materials 0.000 claims abstract description 7
- 238000010000 carbonizing Methods 0.000 claims abstract 3
- 238000000465 moulding Methods 0.000 claims abstract 3
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 17
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 16
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
- 238000010304 firing Methods 0.000 claims description 2
- 235000012239 silicon dioxide Nutrition 0.000 claims description 2
- 239000000377 silicon dioxide Substances 0.000 claims description 2
- 239000000758 substrate Substances 0.000 claims 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical group [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 abstract description 17
- 230000003647 oxidation Effects 0.000 abstract description 5
- 238000007254 oxidation reaction Methods 0.000 abstract description 5
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 4
- 229910052760 oxygen Inorganic materials 0.000 abstract description 4
- 239000001301 oxygen Substances 0.000 abstract description 4
- 230000035939 shock Effects 0.000 abstract description 4
- 239000003575 carbonaceous material Substances 0.000 description 7
- 230000000052 comparative effect Effects 0.000 description 6
- 229910052799 carbon Inorganic materials 0.000 description 5
- 239000006260 foam Substances 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 229910052751 metal Inorganic materials 0.000 description 5
- 239000002184 metal Substances 0.000 description 5
- 239000000919 ceramic Substances 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 229910052878 cordierite Inorganic materials 0.000 description 3
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 3
- 239000003350 kerosene Substances 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 230000008018 melting Effects 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- 239000003245 coal Substances 0.000 description 2
- 230000001747 exhibiting effect Effects 0.000 description 2
- 239000012535 impurity Substances 0.000 description 2
- 150000002739 metals Chemical class 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 2
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- KZHJGOXRZJKJNY-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Si]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O KZHJGOXRZJKJNY-UHFFFAOYSA-N 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- -1 etc. are used Substances 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000003502 gasoline Substances 0.000 description 1
- 239000003779 heat-resistant material Substances 0.000 description 1
- 239000003317 industrial substance Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910052863 mullite Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- PIBWKRNGBLPSSY-UHFFFAOYSA-L palladium(II) chloride Chemical compound Cl[Pd]Cl PIBWKRNGBLPSSY-UHFFFAOYSA-L 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- 230000004580 weight loss Effects 0.000 description 1
Landscapes
- Chimneys And Flues (AREA)
- Catalysts (AREA)
Abstract
Description
【発明の詳細な説明】
〔産業上の利用分野〕
本発明は燃焼触媒に関し、更に詳しくはガスタービン燃
焼コンパスタ−、ボイラの低ＮＯｘ化燃焼用、自動車排
ガス浄化（ガソリン車、ＣＯ／Ｈ１化、ディーゼル車、
カーボンスーツ等）用及び航空機及び飛昇体用エンジン
の失火防止用触媒に関する。DETAILED DESCRIPTION OF THE INVENTION [Field of Industrial Application] The present invention relates to a combustion catalyst, and more specifically to a gas turbine combustion comparator, boiler combustion for reducing NOx, automobile exhaust gas purification (gasoline vehicles, CO/H1 conversion, Diesel Car,
This invention relates to catalysts for preventing misfires in engines for aircraft and flying objects.
従来、燃焼触媒は金属やセラミックスを基材とした成形
体に白金（Ｐｔ）やパラジウム（Ｐｄ）を担持したもの
が主流である。耐熱性金属としては、高アルミナ含有メ
タル、セラミックスとしてはＭｇＯ，Ａｌ□０３． Ｔ
ｌＯ２結晶性複合酸化物ムライトやコージェライトが知
られている。成形体としてはハニカムや格子状の平行流
担体や発泡体等が適用され、特に微粒子状カーボン質に
は発泡体が有効である。Conventionally, the mainstream combustion catalyst has been one in which platinum (Pt) or palladium (Pd) is supported on a molded body made of metal or ceramic as a base material. Heat-resistant metals include high alumina-containing metals, and ceramics include MgO and Al□03. T
The lO2 crystalline composite oxides mullite and cordierite are known. As the molded body, a honeycomb, lattice-shaped parallel flow carrier, foam, etc. are used, and foams are particularly effective for fine particulate carbonaceous materials.
金属材料は機械的強度、特に靭性に富むが、タングステ
ンを除いては融点が低く、燃焼の条件、空／燃比の制御
がはずれると溶解する場合がある。Metal materials have high mechanical strength, especially toughness, but with the exception of tungsten, they have low melting points and may melt if combustion conditions and air/fuel ratios are not controlled.
その点、セラミックスは１８００℃程度までの高融点を
示すも、熱衝撃性に乏しい。しかも１８００℃では燃焼
触媒の基材として満足できる耐熱性ではない。そのため
、燃焼触媒の実用化のためには、耐熱性を示し、かつ熱
衝撃性に強い触媒担体用基材の開発が望まれている。On this point, although ceramics exhibit a high melting point of up to about 1800°C, they have poor thermal shock resistance. Moreover, at 1800°C, it does not have sufficient heat resistance as a base material for a combustion catalyst. Therefore, in order to put combustion catalysts into practical use, it is desired to develop a base material for a catalyst carrier that exhibits heat resistance and is resistant to thermal shock.
本発明は上記技術水準に迄み、かつ上記要望に応じ、耐
熱性でかつ熱衝撃に強い燃焼触媒を提供しようとするも
のである。The present invention aims to provide a combustion catalyst that is heat resistant and resistant to thermal shock, up to the above-mentioned technical level and in response to the above-mentioned demands.
［課題を解決するだめの手段〕
本発明は
（１） メソフェーズを含有する石油ピッチを成形し
、その後炭化した成形体に炭化珪素を生成させた基材に
、白金及び／又はパラジウムを担持してなることを特徴
とする燃焼触媒、（２） 前記１の基材を焼成して、
表面に二酸化珪素の被膜を形成させた基材に、白金及び
／又はパラジウムを担持してなることを特徴とする燃焼
触媒、
である。[Means for Solving the Problems] The present invention provides (1) a base material in which petroleum pitch containing mesophase is molded, and then platinum and/or palladium is supported on a base material in which silicon carbide is formed in a carbonized molded body. A combustion catalyst characterized in that: (2) the base material of 1 above is fired;
A combustion catalyst characterized in that platinum and/or palladium is supported on a base material on which a silicon dioxide film is formed.
耐熱性もあり、極綽て引張り強度の高い黒鉛構造を示す
炭素質の触媒基材化が本発明の主体である。The main focus of the present invention is to use a carbonaceous catalyst base material that is heat resistant and exhibits a graphite structure with extremely high tensile strength.
黒鉛構造を示す炭素質はいわゆる炭素繊維質と同形体で
あり、本発明の黒鉛構造を示す炭素質は石油ピンチの他
に工業化学的原料、石炭液化物からも合成可能であるが
前者（工業化学的原料）からの炭素質は高価であり、後
者（石炭液化物）は不純か混入するため、高強度の炭素
質を狙う場合、不純物除去が必要となり、かえフて高価
となるた釣、石油ピッチが好ましい。The carbonaceous material exhibiting a graphite structure is isomorphous with so-called carbon fiber material, and the carbonaceous material exhibiting the graphite structure of the present invention can be synthesized from industrial chemical raw materials and coal liquefied products in addition to petroleum pinch, but the former (industrial Carbon from chemical raw materials is expensive, and the latter (liquefied coal) contains impurities or contaminants, so when aiming for high-strength carbon, it is necessary to remove impurities, which makes fishing more expensive. Petroleum pitch is preferred.
黒鉛構造をもつ炭素質は酸素のない条件下では２５００
℃程度の耐熱性を示す。しかし、酸素存在下では炭素質
の表面状態にもよるが４００ｔ程度から減量（酸化）が
始まり、特にＰｔ、 Ｐｄ等触媒活性成分を担持すると
極とて短時間で燃焼し消耗する。Carbon with a graphite structure has a carbon content of 2500 in the absence of oxygen.
Shows heat resistance of around ℃. However, in the presence of oxygen, weight loss (oxidation) starts from about 400 tons, depending on the surface condition of the carbonaceous material, and especially when supporting catalytically active components such as Pt and Pd, it burns and is consumed in a very short time.
この耐熱性炭素質を表面保護のため、本発明では炭化珪
素（ＳｉＣ）化し、触媒基材として供するものであり、
更に耐酸化性をも付与するた釣ＳＩＣの表面を酸化させ
て５ｉＯ７を形成させたものを触媒基材とするものであ
る。In order to protect the surface of this heat-resistant carbonaceous material, in the present invention, it is converted into silicon carbide (SiC) and used as a catalyst base material.
Furthermore, the catalyst base material is made by oxidizing the surface of SIC to form 5iO7, which also provides oxidation resistance.
２５００℃以上の耐熱材である黒鉛化炭素質の表面をＳ
ｉＣ化し、さらにこのＳｉＣからＳｉ（］□の緻密なガ
ラス質被膜の生成により、耐酸化性の賦与を行ない、耐
熱性ならび機械的強度をもつ触媒担体を供し、結果的に
所望される燃焼触媒が提供される。S
By forming a dense glassy film of Si(]□ from this SiC, it imparts oxidation resistance and provides a catalyst carrier with heat resistance and mechanical strength, resulting in the desired combustion catalyst. is provided.
（比較例１）
厚さ５０μの２０Ｃｒ−５Ａｌ−残Ｆｅなる耐熱鋼箔を
４００目／（インチ）２のハニカム形状にした基材に、
塩化白金酸をエタノールに溶解してｐｔとしてｌｖｔ％
担持した。これを５５０ｔにて３時間、Ｈ２還元して触
媒とした。(Comparative Example 1) A heat-resistant steel foil of 20Cr-5Al-residue Fe with a thickness of 50μ was used as a base material in a honeycomb shape with 400 stitches/(inch)2.
Dissolve chloroplatinic acid in ethanol and convert it to lvt% as pt.
carried it. This was reduced to H2 at 550 tons for 3 hours to obtain a catalyst.
市販のコージェライトの４００目／（インチ）２のハニ
カムに金属基材と同様にＰｔ１ｗｔ％を担持した触媒を
調製した。A catalyst was prepared in which 1 wt % of Pt was supported on a commercially available cordierite honeycomb of 400 meshes/(inch) 2 in the same manner as the metal base material.
これらの触媒上に、空気／灯油の化学量論比１．１に混
合したガスを空塔速度（Ｓ、Ｖ、）１０６・ｈ−’、４
５０℃の反応条件で接触させると燃焼熱のため金属基材
もコージェライト基材の触媒も溶融解体した。A gas mixture of air/kerosene at a stoichiometric ratio of 1.1 was placed over these catalysts at a superficial velocity (S, V,) of 106 h-', 4
When brought into contact under reaction conditions of 50°C, both the metal base material and the cordierite base catalyst melted and disintegrated due to the heat of combustion.
（実施例１）
メソフェーズ（光学的異方性相）を５０％含有する石油
ピッチをｎ−ヘキサンを少量加え高圧下で加温し、常温
、常圧下に暴露して発泡体を形成させた。これを徐々に
加熱し脱水素することにより黒鉛化した。(Example 1) Petroleum pitch containing 50% mesophase (optically anisotropic phase) was heated under high pressure by adding a small amount of n-hexane, and exposed to normal temperature and pressure to form a foam. This was gradually heated and dehydrogenated to graphitize it.
この構造体く黒鉛化した発泡体）は空孔率が８３％で通
気性のある連続気孔を有している。This structure (graphitized foam) has a porosity of 83% and has open air-permeable pores.
この炭素構造体に比較例と同様にＰｔを１ｗｔ％担持し
、全く同様の条件にて灯油にて燃焼試験をした。このＰ
ｔを担持しない炭素構造体は窒素気流中では２５００℃
でも何ら変化のない耐熱性材料であるが、ｐｔを担持し
て触媒化した後は、炭素質が酸化され、担持したｐｔは
剥離すると同時に炭素質も燃焼消失した。This carbon structure was loaded with 1 wt% of Pt in the same manner as in the comparative example, and a combustion test was conducted using kerosene under exactly the same conditions. This P
The carbon structure that does not carry t has a temperature of 2500°C in a nitrogen stream.
However, although it is a heat-resistant material that does not change in any way, after PT was supported and catalyzed, the carbonaceous material was oxidized, and the supported PT was exfoliated and the carbonaceous material was also burnt and disappeared.
この炭素構造体を１０００℃で加熱しＳｉＨ，と少量の
空気を接触せしめて炭素構造体表面に８１口を形成させ
た。このＳｉＣは１０００℃にて焼成（使用時でも、触
媒調製時を問わず）すると緻密な５ｉＯ７被膜を形成す
る。このような特性をもつＳｉＣ表面に比較例と同様に
Ｐｔ１ｗｔ％を担持し、１０００℃に焼成し触媒化した
。This carbon structure was heated at 1000° C. to bring SiH into contact with a small amount of air to form 81 openings on the surface of the carbon structure. This SiC forms a dense 5iO7 film when calcined at 1000° C. (regardless of whether during use or during catalyst preparation). Similar to the comparative example, 1 wt % of Pt was supported on the SiC surface having such characteristics, and catalyzed by firing at 1000°C.
これを比較例と同様の条件にて灯油の燃焼を実施したが
、１０分間後でも触媒に燃焼溶融、気散の変化は認めら
れなかった。Kerosene was burned under the same conditions as in the comparative example, but no change in combustion melting or dispersion of the catalyst was observed even after 10 minutes.
（実施例２）
前記の方法でＳ１Ｃを形成させた炭素構造体に、比較例
と同じ方法（但し、Ｐｄの原料は塩化パラジウム）でＰ
ｄを１ｗｔ％を担持して焼成した触媒を試作し、燃焼テ
ストを実施した。Ｐｄの場合は４００℃以上の反応温度
で充分燃焼し、Ｐｄの場合と同様全く支障はなかった。(Example 2) P was added to the carbon structure in which S1C was formed by the above method using the same method as in the comparative example (however, the raw material for Pd was palladium chloride).
A prototype catalyst was prepared by supporting 1 wt% of d and a combustion test was conducted. In the case of Pd, sufficient combustion occurred at a reaction temperature of 400° C. or higher, and there were no problems at all as in the case of Pd.
（実施例３）
Ｐｔ （０，５ｗｔ％） 十Ｐｄ （０，５ｗｔ％）を
、表面にＳｉＣを形成させた炭素構造体に担持して焼成
した後、比較例と同様な条件で触媒化し、燃焼テストし
た。この触媒も燃焼は４００℃で充分続行し、Ｐｄの場
合と同様全く支障はなかった。(Example 3) After Pt (0.5 wt%) and Pd (0.5 wt%) were supported on a carbon structure with SiC formed on the surface and fired, catalyzed under the same conditions as in the comparative example, I did a combustion test. This catalyst also continued to burn sufficiently at 400° C., and there were no problems at all as in the case of Pd.
本発明のメソフェーズを含有する石油ピッチを炭素構造
体とし、この構造体にＳｉＣを形成させた基材、または
このＳｉＣの表面を５ｉｎ２にした基材よりなる触媒は
、耐熱性、耐酸化性を賦与し、ガスタービンに適用すれ
ば低ＮＯｘ燃焼を可能とする。また、ボイラーのバーナ
ー邪に適用しても低ＮＯｘ燃焼を可能とする。The catalyst of the present invention, which is made of a base material in which petroleum pitch containing mesophase is used as a carbon structure and SiC is formed on this structure, or a base material in which the surface of this SiC is 5in2, has excellent heat resistance and oxidation resistance. When applied to gas turbines, low NOx combustion is possible. Furthermore, even when applied to boiler burners, low NOx combustion is possible.
さらに、ディーゼルエンジンの排ガス中に本発明の発泡
体構造物を基材とする触媒を採用すれば未燃カーボンの
捕集や捕集した微粒子の再燃焼を可能にする。さらに航
空気のエンジンに採用しておけば、万一失火した場合で
も再着火に効果がある。Furthermore, if a catalyst based on the foam structure of the present invention is employed in the exhaust gas of a diesel engine, it becomes possible to collect unburned carbon and re-burn the collected particulates. Furthermore, if used in aviation engines, it will be effective in re-igniting the fire in the event of a misfire.
Claims (2)
の後炭化した成形体に炭化珪素を生成させた基材に、白
金及び／又はパラジウムを担持してなることを特徴とす
る燃焼触媒。(1) A combustion catalyst characterized in that platinum and/or palladium is supported on a base material formed by molding petroleum pitch containing mesophase and then carbonizing it to form silicon carbide.
被膜を形成させた基材に、白金及び／又はパラジウムを
担持してなることを特徴とする燃焼触媒。(2) A combustion catalyst characterized in that platinum and/or palladium is supported on a substrate obtained by firing the substrate according to claim 1 to form a silicon dioxide film on the surface.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP27938990A JP2831117B2 (en) | 1990-10-19 | 1990-10-19 | Combustion catalyst |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP27938990A JP2831117B2 (en) | 1990-10-19 | 1990-10-19 | Combustion catalyst |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH04156947A true JPH04156947A (en) | 1992-05-29 |
| JP2831117B2 JP2831117B2 (en) | 1998-12-02 |
Family
ID=17610450
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP27938990A Expired - Lifetime JP2831117B2 (en) | 1990-10-19 | 1990-10-19 | Combustion catalyst |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2831117B2 (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2012024745A (en) * | 2010-07-28 | 2012-02-09 | Hitachi Ltd | Catalyst material and method of manufacturing the same |
-
1990
- 1990-10-19 JP JP27938990A patent/JP2831117B2/en not_active Expired - Lifetime
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2012024745A (en) * | 2010-07-28 | 2012-02-09 | Hitachi Ltd | Catalyst material and method of manufacturing the same |
| EP2413406A3 (en) * | 2010-07-28 | 2015-05-13 | Hitachi Ltd. | Catalyst material and method of manufacturing the same |
Also Published As
| Publication number | Publication date |
|---|---|
| JP2831117B2 (en) | 1998-12-02 |
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