CN1623657A - Sosoloid catalyst of methyl alkyl catalyzing burned and its preparation process - Google Patents
Sosoloid catalyst of methyl alkyl catalyzing burned and its preparation process Download PDFInfo
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- CN1623657A CN1623657A CN 200310119324 CN200310119324A CN1623657A CN 1623657 A CN1623657 A CN 1623657A CN 200310119324 CN200310119324 CN 200310119324 CN 200310119324 A CN200310119324 A CN 200310119324A CN 1623657 A CN1623657 A CN 1623657A
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Abstract
A solid solution catalyst for the catalytic combustion of methane in air with low combustion temp (395-570 deg.C) is prepared from cerium oxide and cobalt oxide by urea combustion method.
Description
Technical field
The present invention relates to a kind of Catalysts and its preparation method of methane low-temperature catalytic burning.
Background technology
Natural gas is because characteristics such as its reserves are abundant, cheap, it is little to pollute, thermal efficiency height are described as the clean energy resource of new generation of alternative coal and oil.But the ignition temperature of its main component methane very high (1600 ℃), thereby efficiency of combustion is lower, and in combustion process, can produce minor N O
XWith the imperfect combustion product, thereby cause environmental pollution.Catalytic combustion is just studied widely as a kind of new method of using energy source.Catalytic combustion can reduce the ignition temperature of lower carbon number hydrocarbons, reduces the generation of pernicious gas, and easy control of reaction conditions.Simultaneously, lower ignition temperature also can be avoided the sintering of catalyst itself, thereby efficient and stable good catalyst becomes the key of methane catalytic combustion.
At present, it is the most general with carried noble metal (active component is noble metals such as Pt, Pd, Rh), Ca-Ti ore type composite metal oxide and carrier-borne transition metal catalysts to be used for the catalyst of methane catalytic combustion.Carried noble metal is the best methyl hydride combustion catalyst of present performance, but this class catalyst costs an arm and a leg, and heat endurance is relatively poor, is difficult to large-scale application.Ca-Ti ore type composite metal oxide and carrier-borne transition metal catalysts have higher heat endurance, but its low-temperature catalytic activity is bad.
Ce (CeO
2) because its outstanding redox property and oxygen storage capacity are widely used in the multiple reaction, the auxiliary agent of stablizing noble metal as conduct is used to steam reforming reaction, because of its high oxygen storage power is used to oxygen deprivation and oxygen-enriched combusting reaction etc.Co also often is used to the methane catalytic combustion reaction as catalyst activity composition commonly used.Tian-Cun Xiao etc. are at Journalof Molecular Catalysis A:Chemical (2001 (175): reported ZrO 111-123)
2, MgO, Al
2O
3The situation that is used for methane catalytic combustion etc. carrier loaded Co catalyst, Sheng-Fu Ji etc. are at Catalysis Letters (2001 (75): reported 65-71) that the Co-Mg solid solution catalyst is used for the correlative study of methane catalytic combustion, these catalyst all demonstrate catalytic performance preferably, but low temperature active is still bad.
Summary of the invention
The object of the present invention is to provide a kind of Catalysts and its preparation method of effective catalytic methane burning, when this catalyst is used for the methane catalytic combustion reaction, in lower temperature with the complete catalytic combustion of methane.
The catalyst activity component of the present invention's narration is made up of cerium oxide and cobalt oxide, and the catalyst general formula is: Ce
1-XCo
XO
2, wherein X is 0.10～1.0.
Catalyst activity component of the present invention is made up of cerium oxide and cobalt oxide, and the catalyst general formula is: Ce
1-XCo
XO
2, wherein the x preferable range is 0.20～0.80.
Catalyst preparation process of the present invention is as follows: press general formula Ce
1-XCo
XO
2, wherein X is 0.10～1.0, takes by weighing Ce (NO
3)
26H
2O, Co (NO
3)
26H
2O mixes, and adds 0.5-4.0 times of urea of above-mentioned salt weight, places mortar to grind and obtains pastel, after 10-13 hour, in 500-800 ℃ of roasting 3-6 hour, makes finished catalyst 150-200 ℃ of baking then.
The catalyst of the present invention's narration is used for the methane catalytic combustion reaction, has obtained result preferably.At air and methane volume ratio is 49, and the total air speed of gas is 30000h
-1Condition under can 470 ℃ with methane completing combustion, the total air speed of gas is 5000h
-1Can be under the condition at 395 ℃ with methane completing combustion.(2001 (75): 65-71) institute's results reported is compared, and not only completing combustion temperature reduces more, and initiation temperature is also lower with document Catalysis Letters.
Methane catalytic combustion catalyst provided by the invention compared with prior art has following essential characteristics:
1. catalyst is to be the solid solution catalyst of active component with cerium oxide, cobalt oxide, and the active component content height is cheap.
2. catalyst adopts air as oxidant in the methane catalytic combustion course of reaction, and initiation temperature is low, and the completing combustion temperature is low.
3. catalyst adopts the preparation of burning urea method, the simple easy operating of preparation method, and active component is uniformly dispersed, and has good stability.
The specific embodiment
Embodiment 1: take by weighing 8.7gCe (NO
3)
26H
2O, 1.5gCo (NO
3)
26H
2O puts into mortar and grinds 10～30min, takes by weighing 20g urea again, adds in the mortar to grind 0.5～1.5h, obtains pastel.Pastel is moved in the crucible, put into baking oven, be transferred to groom's stove, make Ce in 500 ℃ of roasting 4h in air in 200 ℃ of baking 12h
0.80Co
0.20O
2Solid solution catalyst.This catalyst is at Air/CH
4=49, the total air speed of gas is 30000h
-1, catalyst amount is that catalytic perfomance is as follows under the condition of 0.2g:
| Temperature (℃) | ????350 | ????450 | ????500 | ????540 | ????560 | ????570 |
| CH 4Conversion ratio (%) | ????2.51 | ????25.68 | ????60.88 | ????87.56 | ????95.04 | ????100 |
Embodiment 2: take by weighing 6.5gCe (NO
3)
26H
2O, 2.9gCo (NO
3)
26H
2O puts into mortar and grinds 10～30min, takes by weighing 20g urea again, adds in the mortar to grind 0.5～1.5h, obtains pastel.The oven dry of catalyst and roasting make Ce with embodiment 1
0.60Co
0.40O
2Solid solution catalyst.This catalyst is at Air/CH
4=49, the total air speed of gas is 30000h
-1, catalyst amount is that catalytic perfomance is as follows under the condition of 0.2g:
| Temperature (℃) | ????350 | ????400 | ????450 | ????480 | ????490 | ????500 |
| CH 4Conversion ratio (%) | ????5.82 | ????21.00 | ????48.41 | ????77.29 | ????89.46 | ????100 |
Embodiment 3: take by weighing 8.7gCe (NO
3)
26H
2O, 5.8gCo (NO
3)
26H
2O puts into mortar and grinds 10～30min, takes by weighing 30g urea again, adds in the mortar to grind 0.5～1.5h, obtains pastel.The oven dry of catalyst and roasting make Ce with embodiment 1
0.50Co
0.50O
2Solid solution catalyst.This catalyst is at Air/CH
4=49, the total air speed of gas is 30000h
-1, catalyst amount is that catalytic perfomance is as follows under the condition of 0.2g:
| Temperature (℃) | ??300 | ??400 | ??450 | ??500 | ??510 | ??520 |
| CH 4Conversion ratio (%) | ??5.37 | ??28.99 | ??61.90 | ??93.26 | ??97.11 | ??100 |
Embodiment 4: take by weighing 5.8gCe (NO
3)
26H
2O, 5.8gCo (NO
3)
26H
2O puts into mortar and grinds 10～30min, takes by weighing 25g urea again, adds in the mortar to grind 0.5～1.5h, obtains pastel.The oven dry of catalyst and roasting make Ce with embodiment 1
0.40Co
0.60O
2Solid solution catalyst.This catalyst is at Air/CH
4=49, the total air speed of gas is 30000h
-1, catalyst amount is that catalytic perfomance is as follows under the condition of 0.2g:
| Temperature (℃) | ??300 | ??350 | ??400 | ??450 | ??480 | ????490 |
| CH 4Conversion ratio (%) | ??5.24 | ??19.77 | ??46.29 | ??81.94 | ??97.75 | ????100 |
Embodiment 5: take by weighing 17.4gCe (NO
3)
26H
2O, 46.6gCo (NO
3)
26H
2O puts into mortar and grinds 10～30min, takes by weighing 120 urea again, adds in the mortar to grind 0.5～1.5h, obtains pastel.The oven dry of catalyst and roasting make Ce with embodiment 1
0.20Co
0.80O
2Solid solution catalyst.This catalyst is at Air/CH
4=49, the total air speed of gas is 30000h
-1, catalyst amount is that catalytic perfomance is as follows under the condition of 0.2g:
| Temperature (℃) | ??300 | ??350 | ??400 | ??420 | ??450 | ????470 |
| CH 4Conversion ratio (%) | ??6.87 | ??26.24 | ??58.55 | ??72.94 | ??91.56 | ????100 |
Embodiment 6: Preparation of catalysts, oven dry and roasting make Ce with embodiment 5
0.20Co
0.80O
2Solid solution catalyst.This catalyst is at Air/CH
4=49, catalyst amount is 0.2g, and catalytic perfomance is as follows under the total air speed condition of gas with various:
Temperature (℃)
Air speed (h
-1)
T
(transforming 10%)T
(transforming 90%)
5000?????????????????265???????????????????????380
10000????????????????280???????????????????????395
15000????????????????285???????????????????????410
20000????????????????310???????????????????????435
30000????????????????315???????????????????????450
Claims (3)
1. the solid solution catalyst of a methane catalytic combustion is characterized in that the catalyst activity component is made up of cerium oxide and cobalt oxide, and the catalyst general formula is: Ce
1-XCo
XO
2, wherein x is 0.10～1.0.
2. catalyst as claimed in claim 1 is characterized in that the catalyst general formula is: Ce
1-XCo
XO
2, wherein x is 0.20～0.8.
3. Preparation of catalysts method according to claim 1 is characterized in that by general formula Ce
1-XCo
XO
2, wherein x is 0.10～1.0, takes by weighing Ce (NO
3)
26H
2O, Co (NO
3)
26H
2O mixes, and adds 0.5-4.0 times of urea of above-mentioned salt weight, places mortar to grind and obtains pastel, after 10-13 hour, in 500-800 ℃ of roasting 3-6 hour, makes finished catalyst 150-200 ℃ of baking then.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 200310119324 CN1623657A (en) | 2003-12-04 | 2003-12-04 | Sosoloid catalyst of methyl alkyl catalyzing burned and its preparation process |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 200310119324 CN1623657A (en) | 2003-12-04 | 2003-12-04 | Sosoloid catalyst of methyl alkyl catalyzing burned and its preparation process |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN1623657A true CN1623657A (en) | 2005-06-08 |
Family
ID=34761339
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN 200310119324 Pending CN1623657A (en) | 2003-12-04 | 2003-12-04 | Sosoloid catalyst of methyl alkyl catalyzing burned and its preparation process |
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| Country | Link |
|---|---|
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101293201B (en) * | 2008-05-30 | 2010-07-28 | 内蒙古大学 | Method for preparing methyl hydride combustion catalyst |
| CN107185545A (en) * | 2017-06-20 | 2017-09-22 | 内蒙古大学 | A kind of copper cobalt doped catalyst preparation and for methane catalytic combustion reaction process |
| CN107282052A (en) * | 2017-06-20 | 2017-10-24 | 内蒙古大学 | A kind of preparation of nickel Zr catalyst and the technique reacted for methane catalytic combustion |
| CN107282051A (en) * | 2017-06-20 | 2017-10-24 | 内蒙古大学 | A kind of preparation of cobalt cerium catalyst and the technique reacted for methane catalytic combustion |
| CN109908910A (en) * | 2017-12-13 | 2019-06-21 | 湖南大学 | Persulfate composite activating agent and its preparation method and application |
-
2003
- 2003-12-04 CN CN 200310119324 patent/CN1623657A/en active Pending
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101293201B (en) * | 2008-05-30 | 2010-07-28 | 内蒙古大学 | Method for preparing methyl hydride combustion catalyst |
| CN107185545A (en) * | 2017-06-20 | 2017-09-22 | 内蒙古大学 | A kind of copper cobalt doped catalyst preparation and for methane catalytic combustion reaction process |
| CN107282052A (en) * | 2017-06-20 | 2017-10-24 | 内蒙古大学 | A kind of preparation of nickel Zr catalyst and the technique reacted for methane catalytic combustion |
| CN107282051A (en) * | 2017-06-20 | 2017-10-24 | 内蒙古大学 | A kind of preparation of cobalt cerium catalyst and the technique reacted for methane catalytic combustion |
| CN109908910A (en) * | 2017-12-13 | 2019-06-21 | 湖南大学 | Persulfate composite activating agent and its preparation method and application |
| CN109908910B (en) * | 2017-12-13 | 2020-05-19 | 湖南大学 | Persulfate composite activator and preparation method and application thereof |
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