JPS63162042A - Catalyst for contact combustion - Google Patents
Catalyst for contact combustionInfo
- Publication number
- JPS63162042A JPS63162042A JP61308559A JP30855986A JPS63162042A JP S63162042 A JPS63162042 A JP S63162042A JP 61308559 A JP61308559 A JP 61308559A JP 30855986 A JP30855986 A JP 30855986A JP S63162042 A JPS63162042 A JP S63162042A
- Authority
- JP
- Japan
- Prior art keywords
- catalyst
- palladium
- alumina carrier
- alumina
- contact combustion
- 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
- 239000003054 catalyst Substances 0.000 title claims abstract description 48
- 238000002485 combustion reaction Methods 0.000 title abstract description 9
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims abstract description 52
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 33
- 229910052763 palladium Inorganic materials 0.000 claims abstract description 25
- 238000007084 catalytic combustion reaction Methods 0.000 claims description 13
- 230000006866 deterioration Effects 0.000 abstract description 8
- PIBWKRNGBLPSSY-UHFFFAOYSA-L palladium(II) chloride Chemical compound Cl[Pd]Cl PIBWKRNGBLPSSY-UHFFFAOYSA-L 0.000 abstract description 6
- 238000000151 deposition Methods 0.000 abstract 1
- 230000000052 comparative effect Effects 0.000 description 11
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 8
- 238000000034 method Methods 0.000 description 6
- 239000004480 active ingredient Substances 0.000 description 5
- 230000000694 effects Effects 0.000 description 5
- 239000002344 surface layer Substances 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- 230000003197 catalytic effect Effects 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000007796 conventional method Methods 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 239000010410 layer Substances 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Chemical compound [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical group N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 1
- 229910000873 Beta-alumina solid electrolyte Inorganic materials 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000004453 electron probe microanalysis Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 230000008020 evaporation Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- WHOPEPSOPUIRQQ-UHFFFAOYSA-N oxoaluminum Chemical compound O1[Al]O[Al]1 WHOPEPSOPUIRQQ-UHFFFAOYSA-N 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 150000002941 palladium compounds Chemical class 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 235000010344 sodium nitrate Nutrition 0.000 description 1
- 239000004317 sodium nitrate Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Landscapes
- Catalysts (AREA)
Abstract
Description
【発明の詳細な説明】
［産業上の利用分野）
本発明は、パラジウムをアルミナ担体内部まで均一に担
持させることにより、耐熱性を向上させた接触燃焼用触
媒に関する。DETAILED DESCRIPTION OF THE INVENTION [Field of Industrial Application] The present invention relates to a catalyst for catalytic combustion that has improved heat resistance by uniformly supporting palladium inside an alumina carrier.
接触燃焼用触媒として、一般に、（１）点火温度が低い
こと、（２）燃焼継続に必要な予熱温度が低いこと、（
３）容積燃焼率が高いこと、（４）触媒表面での燃焼が
均一であること、（５）汚染物質の排出量が少ないこと
、（６）多様な燃料が使用可能なこと等の特性が要求さ
れる。Catalytic combustion catalysts generally have (1) low ignition temperature, (2) low preheating temperature required for continued combustion, (
3) high volumetric combustion rate, (4) uniform combustion on the catalyst surface, (5) low pollutant emissions, and (6) ability to use a variety of fuels. required.
従来、このような特性が要求される接触燃焼用触媒、特
にメタン燃焼用触媒としては、Ｐｄ／ＡＪ２ ０３
、Ｐｄ ／Ｔｉ ０２ 、Ｐｔ ／Ｓｉ ０
２ ・Ａｌ２Ｏ２、Ｐｊ／ＡＪ２０３等が用いられ、
これら触媒は高い触媒性能を有することが知られている
。Conventionally, Pd/AJ2 03 has been used as a catalyst for catalytic combustion, especially for methane combustion, which requires such characteristics.
, Pd /Ti 02 , Pt /Si 0
2 ・Al2O2, Pj/AJ203, etc. are used,
These catalysts are known to have high catalytic performance.
しかし、これらの触媒は、高温下で長時間使用されると
、触媒が熱劣化し、触媒性能が低下するという問題があ
った。However, when these catalysts are used at high temperatures for long periods of time, they suffer from thermal deterioration, resulting in a decrease in catalyst performance.
この高温下での触媒の熱劣化対策として、アルミナ等の
担体にアルカリ土類や希土類酸化物を添加し、担体の安
定性を向上させる方法等が提案されており、例えば、Ｙ
−アルミナにランタンを添加する方法、Ｙ−アルミナに
バリウムを添加する方法等である。また、活性成分であ
る貴金属の層を耐熱性酸化物で被覆することにより、貴
金属の蒸発を防止して劣化を防止する方法も提案されて
いる（特開昭５８−３６４１号公報）。As a countermeasure against thermal deterioration of the catalyst at high temperatures, methods have been proposed in which alkaline earth or rare earth oxides are added to a support such as alumina to improve the stability of the support.
- A method of adding lanthanum to alumina, a method of adding barium to Y-alumina, etc. Furthermore, a method has been proposed in which a layer of a noble metal, which is an active ingredient, is coated with a heat-resistant oxide to prevent evaporation of the noble metal and thereby prevent deterioration (Japanese Patent Laid-Open No. 58-3641).
しかしながら、これらのいずれの方法においても高温下
での長時間の使用においては、触媒は熱劣化し、触媒性
能が低下するという問題は避けられなかった。However, in any of these methods, when used for a long time at high temperatures, the catalyst inevitably deteriorates due to heat and the catalyst performance deteriorates.
このように、高温下で、長期に亘って熱劣化を生ぜず、
実用に供し得る接触燃焼用触媒は未だ得られていない。In this way, under high temperatures, there will be no thermal deterioration over a long period of time,
A catalyst for catalytic combustion that can be put to practical use has not yet been obtained.
［発明が解決しようとする問題点］
本発明は、上記従来技術の問題点に鑑みてなされたもの
で、高温下での経時の使用による触媒の劣化を防止し、
高い触媒特性を有する接触燃焼用触媒を提供することを
目的とする。[Problems to be Solved by the Invention] The present invention has been made in view of the above-mentioned problems of the prior art.
An object of the present invention is to provide a catalyst for catalytic combustion that has high catalytic properties.
［問題点を解決するための手段および作用コ本発明者ら
は、上記目的を達成するために鋭意検討した結果、パラ
ジウムのアルミナ担体上への担持状態を制御することに
より、高温接触燃焼用触媒の熱的劣化挙動を緩和するこ
とができることを見い出し、本発明を完成するに至った
。[Means and effects for solving the problem] As a result of intensive studies to achieve the above object, the present inventors have developed a catalyst for high-temperature catalytic combustion by controlling the state of palladium supported on an alumina carrier. It has been discovered that the thermal deterioration behavior of can be alleviated, and the present invention has been completed.
すなわち本発明は、パラジウムをアルミナ担体内部まで
均一に担持させたことを特徴とする接触燃焼用触媒にあ
る。That is, the present invention resides in a catalytic combustion catalyst characterized in that palladium is uniformly supported inside an alumina carrier.
本発明の接触燃焼用触媒の担体であるアルミナとしては
、特に制限はなく、γ−アルミナのみならず、α−アル
ミナ、β−アルミナ等も用いられる。The alumina that is the carrier for the catalytic combustion catalyst of the present invention is not particularly limited, and not only γ-alumina but also α-alumina, β-alumina, etc. can be used.
担体であるアルミナに活性成分であるパラジウムを担持
させる方法としては、特に限定されないが、少なくとも
アルミナ担体内部まで均一にパラジウムが担持されてい
ることが必要である。例えばアルミナ担体に塩化パラジ
ウム等のパラジウム化合物の溶液を滴下または注加して
含浸し、次いで乾燥、還元することによって、本発明の
接触燃焼用触媒が得られる。The method for supporting palladium, which is an active ingredient, on alumina, which is a carrier, is not particularly limited, but it is necessary that palladium is uniformly supported at least to the inside of the alumina carrier. For example, the catalyst for catalytic combustion of the present invention can be obtained by dripping or pouring a solution of a palladium compound such as palladium chloride onto an alumina carrier to impregnate it, followed by drying and reduction.
この触媒の形状は、特に限定されないが、例えば球状、
平板状、多角柱状、ハニカム状等が挙げられる。The shape of this catalyst is not particularly limited, but for example, spherical,
Examples include flat plate shape, polygonal column shape, and honeycomb shape.
この本発明の接触燃焼用触媒の一例を第１図（ａ）に示
す。第１図（ａ）は、球状のアルミナ担体の内部まで活
性成分であるパラジウムを均一に担持させた触媒を示す
断面図である。パラジウムの担持量を一定岱とすると、
一般には、球状のアルミナ担体の表層部にのみパラジウ
ムを担持した第１図（ｂ）に断面が示される触媒または
球状アルミナの中層部までパラジウムを担持した第１図
（Ｃ）に断面が示される触媒のほうが、触媒表面の活性
成分の密度が高く、活性が大きいことから、触媒性能が
高いとされている。An example of the catalytic combustion catalyst of the present invention is shown in FIG. 1(a). FIG. 1(a) is a cross-sectional view showing a catalyst in which palladium, an active ingredient, is uniformly supported inside a spherical alumina carrier. Assuming that the amount of palladium supported is constant,
In general, the cross section of the catalyst is shown in Figure 1 (b) in which palladium is supported only on the surface layer of a spherical alumina carrier, or the cross section is shown in Figure 1 (C) in which palladium is supported up to the middle layer of spherical alumina carriers. Catalysts are said to have higher catalytic performance because the density of active components on the surface of the catalyst is higher and the activity is greater.
しかし、接触燃焼反応のように触媒が高温下の雰囲気に
長時間曝されるような場合には、第１図（ａ）に示した
担持状態の方が耐熱劣化性に対して効果がある。このよ
うな活性成分であるパラジウムの担持状態による熱的劣
化挙動に対する効果は、これまで知見されていない。However, in cases where the catalyst is exposed to a high-temperature atmosphere for a long period of time, such as in a catalytic combustion reaction, the supported state shown in FIG. 1(a) is more effective in terms of thermal deterioration resistance. The effect of the supported state of palladium, which is an active ingredient, on thermal deterioration behavior has not been known so far.
［実施例］
以下、実施例、比較例および実験例に基づいて本発明を
さらに具体的に説明する。[Examples] Hereinafter, the present invention will be described in more detail based on Examples, Comparative Examples, and Experimental Examples.
実施例１
球状アルミナ担体く５履φ、吸水率０．４５ ＣＣ／ｇ
） ｉｏｏｇを５ｏｏｃｃのビーカーに入れてアルミ
ナ担体を振り混ぜながら０．１０４ ｍｏｌ／ Ｊの塩
化パラジウム溶液４５ｃｃをｖ温で滴下しながら含浸し
た。しかる後、常法により乾燥器で乾燥し、電気炉にて
水素流通下で２５０℃、３時間還元してパラジウム含有
量０．５型理％の触媒Ａを得た。Example 1 Spherical alumina carrier 5 mm diameter, water absorption rate 0.45 CC/g
) ioog was placed in a 50cc beaker and the alumina support was impregnated with 45cc of 0.104 mol/J palladium chloride solution dropwise at V temperature while shaking. Thereafter, it was dried in a dryer using a conventional method, and reduced in an electric furnace at 250° C. for 3 hours under flowing hydrogen to obtain catalyst A having a palladium content of 0.5%.
このようにして調製された触媒Ａのアルミナ担体上での
パラジウムの分布状態をＸ線マイクロアナライザー（Ｅ
ＰＭＡ）で測定した結果、パラジウムはアルミナ担体の
全層部に担持されていることがわかった。The distribution state of palladium on the alumina support of catalyst A prepared in this way was measured using an X-ray microanalyzer (E
As a result of measurement using PMA), it was found that palladium was supported in all layers of the alumina carrier.
比較例１
実施例１の触媒Ａの調製で使用したものと同様のアルミ
ナ担体１００ｇを５００ｃｃのビーカーに入れ０．４１
ｍｏｌ／ Ｊの硝酸ナトリウム溶液４５ＣＣを室温で滴
下しながら含浸した。常法により乾燥し、電気炉にて空
気流通下で５００℃、３時間焼成した。この担体に０．
１０４ ｍｏｌ／Ｊの塩化パラジウム溶液４５ＣＣを実
施例１と同様に滴下しながら含浸した。常法により乾燥
器で乾燥し、電気炉にて水素流通下２５０℃、３時間還
元して触媒Ｂを得た。Comparative Example 1 100 g of alumina support similar to that used in the preparation of catalyst A in Example 1 was placed in a 500 cc beaker and the amount of 0.41
45 CC of mol/J sodium nitrate solution was impregnated dropwise at room temperature. It was dried by a conventional method and fired in an electric furnace at 500° C. for 3 hours under air circulation. This carrier has 0.
45 CC of a 104 mol/J palladium chloride solution was dropped and impregnated in the same manner as in Example 1. The mixture was dried in a dryer using a conventional method, and reduced in an electric furnace at 250° C. under hydrogen flow for 3 hours to obtain catalyst B.
このようにして調製された触媒Ｂは、Ｅ ＰＭＡで測定
した結果、パラジウムがアルミナ担体表層部から約１１
ｎＩＲのところまで担持されていることがわかった。Catalyst B prepared in this manner was measured by E PMA, and palladium was found to be about 11% from the surface layer of the alumina support.
It was found that it was carried up to the nIR.
比較例２
比較例１の触媒Ｂの調製で使用したものと同じｆｌＩＩ
！Ｉナトリウム溶液の濃度を１．Ｏｍｏｌ／Ｊに変えて
、その４５ｃｃを担体アルミナ１００ｇに含浸した。こ
の担体に０．１０４ ｍｏｌ／Ｊの塩化パラジウム溶液
４５ＣＣを実施例１と同様に滴下しながら含浸して触媒
Ｃを得た。Comparative Example 2 Same flII as used in the preparation of catalyst B of Comparative Example 1
! The concentration of sodium I solution is 1. The amount was changed to Omol/J, and 45 cc of the solution was impregnated into 100 g of carrier alumina. This carrier was impregnated with 45 CC of a 0.104 mol/J palladium chloride solution dropwise in the same manner as in Example 1 to obtain catalyst C.
このようにして調製された触媒Ｃを、Ｅ ＰＭＡで測定
した結果、パラジウムがアルミナ担体表層部から約０．
２ｍｍのところまで担持されていることがわかった。As a result of measuring the catalyst C prepared in this manner by E PMA, it was found that palladium was approximately 0.0% palladium from the surface layer of the alumina support.
It was found that the particles were supported up to a depth of 2 mm.
比較例３
実施例１の触ｔｓＡの調製で使用したものと同じアルミ
ナ担体１００ｇを２００℃に加熱しながら ０．１０４
ｍｏｌ／Ｊの塩化パラジウム溶液４５ｃｃを含浸し、乾
燥後、電気炉にて水素流通下で２５０℃、３時間還元し
て触媒りを得た。Comparative Example 3 While heating 100 g of the same alumina support used in the preparation of tsA in Example 1 to 200°C, 0.104
It was impregnated with 45 cc of a mol/J palladium chloride solution, dried, and then reduced in an electric furnace at 250° C. for 3 hours under hydrogen flow to obtain a catalyst.
このようにして調製された触媒りは、ＥＰＭＡで測定し
た結果、比較例１の触ＩＢと同様にパラジウムがアルミ
ナ担体表層部から約１Ｍのところまで担持されているこ
とがわかった。The thus prepared catalyst was measured by EPMA, and it was found that palladium was supported up to about 1M from the surface layer of the alumina carrier, similar to Comparative Example 1.
実験例
実施例１および比較例１〜３で調製されたＡ〜Ｄの各触
媒を電気炉にて８００℃および１１００℃で２４時間熱
処理した。このようにして得られた熱処理触媒を用いて
、下記の条件でメタン燃焼反応を行ない、メタン変換率
５０％を得るのに必要な反応温度を評価した。反応条件
としては、メタンガス濃度５．７％、酸素濃度１９．８
％、および残部を窒素ガスとし、空間速度を１２０００
Ｈｒ−１で行なった。結果を第１表に示した。Experimental Examples Each of the catalysts A to D prepared in Example 1 and Comparative Examples 1 to 3 was heat treated in an electric furnace at 800°C and 1100°C for 24 hours. Using the heat-treated catalyst thus obtained, a methane combustion reaction was carried out under the following conditions, and the reaction temperature required to obtain a methane conversion rate of 50% was evaluated. The reaction conditions were a methane gas concentration of 5.7% and an oxygen concentration of 19.8%.
%, and the balance is nitrogen gas, and the space velocity is 12000.
The test was carried out using Hr-1. The results are shown in Table 1.
第１表
第１表の結果より、熱処理に対して安定な活性を示す順
序は、実施例１（触媒Ａ）、比較例１（ＭｉＢ）、比較
例３（触媒Ｄ）、比較例２（触媒Ｃ）となった。Table 1 From the results in Table 1, the order of stable activity against heat treatment is Example 1 (Catalyst A), Comparative Example 1 (MiB), Comparative Example 3 (Catalyst D), and Comparative Example 2 (Catalyst C).
この結果から、本発明の触媒Ａ（実施例１）は、触媒Ｂ
〜Ｄ（比較例１〜３）に比較して耐熱性に優れているこ
とがわかる。From this result, catalyst A of the present invention (Example 1) was found to be
It can be seen that the heat resistance is excellent compared to ~D (Comparative Examples 1 to 3).
Ｕ発明の効果Ｊ
以上説明したように、活性成分であるパラジウムをアル
ミナ担体内部まで均一に担持させた本発明によれば、接
触燃焼用触媒の耐熱性を大幅に向上することができる。Effects of the Invention J As explained above, according to the present invention in which palladium, which is an active ingredient, is uniformly supported inside the alumina carrier, the heat resistance of the catalyst for catalytic combustion can be greatly improved.
第１図（ａ＞〜（Ｃ）は、パラジウムのアルミナ担体へ
の担持状態を示す断面図である。
特許出願人 日 揮 株 式 会 社代理
人 弁理士 伊 東 辰 雄
代理人 弁理士 伊 東 哲 也
第１図Figures 1 (a> to (C)) are cross-sectional views showing the state of palladium supported on an alumina carrier. Patent applicant: JGC Corporation Company representative: Patent attorney: Tatsuo Ito: Patent attorney: Tatsuo Ito Tetsuya Figure 1
Claims (1)
たことを特徴とする接触燃焼用触媒。1. A catalyst for catalytic combustion characterized by having palladium uniformly supported inside an alumina carrier.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP61308559A JPS63162042A (en) | 1986-12-26 | 1986-12-26 | Catalyst for contact combustion |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP61308559A JPS63162042A (en) | 1986-12-26 | 1986-12-26 | Catalyst for contact combustion |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS63162042A true JPS63162042A (en) | 1988-07-05 |
Family
ID=17982487
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP61308559A Pending JPS63162042A (en) | 1986-12-26 | 1986-12-26 | Catalyst for contact combustion |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS63162042A (en) |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5662542A (en) * | 1979-10-29 | 1981-05-28 | Osaka Gas Co Ltd | Production of catalyst body for combustion |
| JPS6014938A (en) * | 1983-07-06 | 1985-01-25 | Toshiba Corp | Combustion catalyst for gas turbine |
-
1986
- 1986-12-26 JP JP61308559A patent/JPS63162042A/en active Pending
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5662542A (en) * | 1979-10-29 | 1981-05-28 | Osaka Gas Co Ltd | Production of catalyst body for combustion |
| JPS6014938A (en) * | 1983-07-06 | 1985-01-25 | Toshiba Corp | Combustion catalyst for gas turbine |
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