CN1049611C - Ceramic fibre loaded high temperature reaction catalyst - Google Patents
Ceramic fibre loaded high temperature reaction catalyst Download PDFInfo
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- CN1049611C CN1049611C CN93103356A CN93103356A CN1049611C CN 1049611 C CN1049611 C CN 1049611C CN 93103356 A CN93103356 A CN 93103356A CN 93103356 A CN93103356 A CN 93103356A CN 1049611 C CN1049611 C CN 1049611C
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- CN
- China
- Prior art keywords
- ceramic fibre
- high temperature
- catalyst
- temperature reaction
- hours
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
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- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)
- Catalysts (AREA)
Abstract
The present invention belongs to a preparation technique of ceramic fiber supported high temperature reaction catalysts. The present invention indicates that when the consumption of active constituents is only one fourth of or less than the original consumption of catalysts, activity and selectivity higher than those of the original activity and selectivity can also be kept at 650 to 750 DEG C. The addition of ceramic fibers reduces corrosiveness, the loss of the active constituents is suppressed, carbon deposition is avoided or reduced, and the service life of the catalysts is prolonged.
Description
The invention belongs to the technology of preparing of ceramic fibre loaded high temperature reaction catalyst.
The high-temperature catalytic reaction, as: the used catalyst such as exhaustive oxidation of hydrocarbon oxidation, oxidative dehydrogenation, isomerization, hydro carbons, in course of reaction, because reaction temperature height, the temperature distributing disproportionation of catalyst layer is even, often cause phenomenons such as sintering, carbon deposit, the loss of activity of such catalysts component, therefore seriously influenced life of catalyst.Particularly in the reaction of methane oxidation coupling high-temperature catalytic, used catalyst contains alkali metal, alkaline-earth metal etc., and the loss of active component is even more serious.At the problems referred to above, we have found the carrier of the good ceramic fibre of resistance to elevated temperatures as fixed bde catalyst finally through experiment repeatedly, have made ceramic fibre loaded high temperature reaction catalyst.The present invention has following characteristics:
The consumption of active component be original catalyst amount 1/4th or still less, still can keep or be higher than original C at 650～750 ℃
2Active, selectivity.
2. reduced the corrosivity of catalyst, suppressed the loss of active component consersion unit.
The present invention be with catalyst cupport on ceramic fibre, thereby increased the contact area of reaction gas, the active site of catalyst phase is evenly distributed, help catalytic reaction.
4. ceramic fibre itself is high temperature resistant, still keeps its chemical stability after the interpolation, so do not change the character of original catalyst activity component.Because active component is dispersed on the ceramic fibre, so reaction temperature profile is even, avoids or has reduced carbon deposit, thereby prolonged life of catalyst.
5. preparation technology is simple, has reduced cost, has improved economic benefit.
The present invention be with former high temperature reaction catalyst as used catalyst such as hydrocarbon oxidation, oxidative dehydrogenation, isomerization, hydro carbons exhaustive oxidation, methane oxidation couplings, be ground into the following powder of 160 orders, evenly mix with ceramic fibre with water-soaked.The part by weight of raw catalyst and water is 1: 25～35.The weight ratio of raw catalyst and ceramic fibre is: 1: 3～5.The pore volume of ceramic fibre is about 7 milliliters/gram, therefore can make the catalyst granules uniform load on ceramic fibre, ceramic fibre after the load can obtain ceramic fibre loaded high temperature reaction catalyst 800 ℃ of following roastings more than 3 hours 110 ℃ of oven dry 2 hours.Methane oxidation coupling synthesizing ethylene, the used ceramic fibre loaded high temperature reaction catalyst preparation process of ethane are:
At first, with alkali metal such as Li, Na, K, the soluble-salt of alkaline-earth metal such as Mg, Ca, Ba, Sr such as nitrate, carbonate, sulfate, chloride etc. are immersed in rare earth oxide such as La
2O
3, CeO
3, Sm
2O
3On pressed powder.The optimum mole ratio of alkali metal, alkaline-earth metal and rare earth oxide is: (0.5～15): (1～20): (20～50).Dip time preferably about half an hour, was wetting shape more than 10 minutes behind the dipping, 110 ℃ of oven dry about 2 hours, again 450 ℃ of roastings about 3 hours, at last 800 ℃ of roastings more than 4 hours.
Secondly, the catalyst activity component that above-mentioned roasting is good is ground into the powder below 160 orders, get 1 gram and add 30 ml waters, soaking the back mixes with 4 gram ceramic fibres, make catalyst activity component uniform load on ceramic fibre, 110 ℃ of oven dry 2 hours, promptly obtain ceramic fibre loaded high temperature reaction catalyst more than 3 hours 800 ℃ of roastings more then.
The reaction of evaluate catalysts and device: adopt fixed-bed quartz reactor, internal diameter is 6 millimeters, reaction temperature is between 500～800 ℃, and the volume proportion of feed gas methane and oxygen is: (10～3): 1, and the catalytic reaction of employing is methane oxidation coupling system ethene, ethane.
Embodiment
Take by weighing 5 gram La
2O
3, grind; With same La
2O
3Mol ratio be 1: 36 Ba (NO
3)
2The aqueous solution be immersed in La
2O
3Go up afterwards 110 ℃ of oven dry, again with same La
2O
3Mol ratio be: 0.5: 36 K
2SO
4The aqueous solution is immersed in Ba (NO
3)
2～La
2O
3On the solid, 110 ℃ of oven dry 2 hours, promptly get K: Ba: La=0.5 more than 3 hours 800 ℃ of roastings: 1: 36 K then
2SO
4-BaO-La
2O
3Catalyst.Get catalyst (no ceramic fibre loaded) 0.2 gram of above-mentioned preparation, put into the device of evaluate catalysts.In the reaction gas, the volume ratio of methane and oxygen is 7: 1, and overall flow rate is 64 ml/min, under 650～750 ℃ of situations of reaction temperature, and methane conversion, C
2Hydrocarbon yield (C
2=C
2=+C
2 0, C
2=be ethene, C
2 0Be ethane) and C
2During the selectivity of hydrocarbon is listed in the table below:
650 ℃ of 700 ℃ 750 ℃ methane conversions (%), 36.13 35.33 33.30C
2 =Yield (%) 9.72 10.11 9.96C
2 0Yield (%) 9.24 9.26 9.41C
2Yield (%) 18.96 19.36 19.37C
2Hydrocarbon-selective (%) 52.47 54.79 58.16
The K that the front is made then
2SO
4-BaO-La
2O
3Catalyst is ground into below 160 orders, getting 1 gram adds 30 ml waters and soaks back and 4 and restrain ceramic fibres and mix, catalyst is loaded on the ceramic fibre uniformly, 110 ℃ of oven dry 2 hours, promptly make ceramic fibre loaded high temperature reaction catalyst more than 3 hours 800 ℃ of roastings more then.Get 0.2 gram equally, put into catalyst test apparatus, reaction condition is the same, and reaction result is listed following table in:
650 ℃ of 700 ℃ 750 ℃ methane conversions (%), 34.41 33.14 32.92C
2 =Yield (%) 8.41 9.26 10.53C
2 0Yield (%) 9.49 9.76 9.23C
2Yield (%) 17.90 19.02 19.76C
2Hydrocarbon-selective (%) 52.02 57.39 60.02
Claims (2)
1, the preparation method of a kind of methane oxidation coupling synthesizing ethylene, ethane high temperature reaction catalyst, it is characterized in that: be 0.5～15: 1～20 with alkali metal, alkaline-earth metal and rare earth oxide mol ratio at first: 20～50 alkali metal and alkaline-earth metal soluble-salt solution impregnation are on the pressed powder of rare earth oxide, dipping is more than 10 minutes, dried 2 hours down at 110 ℃, 450 ℃ of following roastings 3 hours, promptly make thinner agent active constituent more than 4 hours 800 ℃ of following roastings; Then active constituent is ground into the powder below 160 orders, water-soaked with 25～35 times of weight, ceramic fibre with 3～5 times of active constituent weight evenly mixes again, catalyst granules evenly is loaded on the ceramic fibre, dried 2 hours down at 110 ℃, 800 ℃ of following roastings 3 hours, promptly make ceramic fibre loaded high temperature reaction catalyst.
2, as the preparation method of right 1 described high temperature reaction catalyst, it is characterized in that alkali metal is Li, Na, K, alkaline-earth metal is Mg, Ca, Ba, Sr, rare earth oxide is La
2O
3, CeO
2, Sm
2O
3
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN93103356A CN1049611C (en) | 1993-03-22 | 1993-03-22 | Ceramic fibre loaded high temperature reaction catalyst |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN93103356A CN1049611C (en) | 1993-03-22 | 1993-03-22 | Ceramic fibre loaded high temperature reaction catalyst |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1078922A CN1078922A (en) | 1993-12-01 |
| CN1049611C true CN1049611C (en) | 2000-02-23 |
Family
ID=4984607
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN93103356A Expired - Fee Related CN1049611C (en) | 1993-03-22 | 1993-03-22 | Ceramic fibre loaded high temperature reaction catalyst |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN1049611C (en) |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5057482A (en) * | 1988-12-15 | 1991-10-15 | Matsushita Electric Industrial Co., Ltd. | Catalytic composite for purifying exhaust gases and a method for preparing the same |
| CN1061164A (en) * | 1990-08-21 | 1992-05-20 | 加州大学评议会 | The catalyzed selective oxydehydrogenation of methane |
| CN1061730A (en) * | 1991-11-13 | 1992-06-10 | 厦门大学 | The methane oxidation coupling catalyst for making ethylene |
| CN1062717A (en) * | 1990-12-21 | 1992-07-15 | 埃尼里塞尔什联合股票公司 | With methane conversion is the method and the catalyzer of higher hydrocarbon products |
-
1993
- 1993-03-22 CN CN93103356A patent/CN1049611C/en not_active Expired - Fee Related
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5057482A (en) * | 1988-12-15 | 1991-10-15 | Matsushita Electric Industrial Co., Ltd. | Catalytic composite for purifying exhaust gases and a method for preparing the same |
| CN1061164A (en) * | 1990-08-21 | 1992-05-20 | 加州大学评议会 | The catalyzed selective oxydehydrogenation of methane |
| CN1062717A (en) * | 1990-12-21 | 1992-07-15 | 埃尼里塞尔什联合股票公司 | With methane conversion is the method and the catalyzer of higher hydrocarbon products |
| CN1061730A (en) * | 1991-11-13 | 1992-06-10 | 厦门大学 | The methane oxidation coupling catalyst for making ethylene |
Also Published As
| Publication number | Publication date |
|---|---|
| CN1078922A (en) | 1993-12-01 |
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