CN101628241B - Monolithic catalyst for dimethyl ether catalytic combustion and preparation method and application thereof - Google Patents
Monolithic catalyst for dimethyl ether catalytic combustion and preparation method and application thereof Download PDFInfo
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- CN101628241B CN101628241B CN2009100417998A CN200910041799A CN101628241B CN 101628241 B CN101628241 B CN 101628241B CN 2009100417998 A CN2009100417998 A CN 2009100417998A CN 200910041799 A CN200910041799 A CN 200910041799A CN 101628241 B CN101628241 B CN 101628241B
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- dimethyl ether
- molecular sieve
- manganese oxide
- catalytic combustion
- oxide molecular
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- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical compound COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 title claims abstract description 80
- 238000007084 catalytic combustion reaction Methods 0.000 title claims abstract description 30
- 239000003054 catalyst Substances 0.000 title claims abstract description 23
- 238000002360 preparation method Methods 0.000 title claims abstract description 6
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 claims abstract description 94
- 239000002808 molecular sieve Substances 0.000 claims abstract description 46
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims abstract description 46
- 239000002002 slurry Substances 0.000 claims abstract description 22
- 229910052878 cordierite Inorganic materials 0.000 claims abstract description 11
- 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 claims abstract description 11
- 239000000853 adhesive Substances 0.000 claims abstract description 10
- 230000001070 adhesive effect Effects 0.000 claims abstract description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 12
- 238000013019 agitation Methods 0.000 claims description 10
- 239000008367 deionised water Substances 0.000 claims description 10
- 229910021641 deionized water Inorganic materials 0.000 claims description 10
- 238000007598 dipping method Methods 0.000 claims description 10
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 6
- 229920001427 mPEG Polymers 0.000 claims description 5
- 239000002202 Polyethylene glycol Substances 0.000 claims description 4
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 4
- 229920001223 polyethylene glycol Polymers 0.000 claims description 4
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 4
- 239000004743 Polypropylene Substances 0.000 claims description 3
- 238000005303 weighing Methods 0.000 claims description 2
- PNVJTZOFSHSLTO-UHFFFAOYSA-N Fenthion Chemical compound COP(=S)(OC)OC1=CC=C(SC)C(C)=C1 PNVJTZOFSHSLTO-UHFFFAOYSA-N 0.000 claims 4
- 239000005416 organic matter Substances 0.000 abstract description 2
- 238000000576 coating method Methods 0.000 abstract 1
- 238000000034 method Methods 0.000 abstract 1
- 239000000203 mixture Substances 0.000 abstract 1
- 239000000919 ceramic Substances 0.000 description 16
- 239000000446 fuel Substances 0.000 description 9
- 238000002485 combustion reaction Methods 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 3
- 239000003915 liquefied petroleum gas Substances 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- KBPLFHHGFOOTCA-UHFFFAOYSA-N 1-Octanol Chemical compound CCCCCCCCO KBPLFHHGFOOTCA-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 239000002283 diesel fuel Substances 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000011572 manganese Substances 0.000 description 2
- IVKNZCBNXPYYKL-UHFFFAOYSA-N 2-[2-[2-[2-[2-[2-[2-[2-[2-[2-[4-(2,4,4-trimethylpentan-2-yl)phenoxy]ethoxy]ethoxy]ethoxy]ethoxy]ethoxy]ethoxy]ethoxy]ethoxy]ethoxy]ethanol Chemical compound CC(C)(C)CC(C)(C)C1=CC=C(OCCOCCOCCOCCOCCOCCOCCOCCOCCOCCO)C=C1 IVKNZCBNXPYYKL-UHFFFAOYSA-N 0.000 description 1
- CIWBSHSKHKDKBQ-JLAZNSOCSA-N Ascorbic acid Chemical compound OC[C@H](O)[C@H]1OC(=O)C(O)=C1O CIWBSHSKHKDKBQ-JLAZNSOCSA-N 0.000 description 1
- 229910015999 BaAl Inorganic materials 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- IMNFDUFMRHMDMM-UHFFFAOYSA-N N-Heptane Chemical compound CCCCCCC IMNFDUFMRHMDMM-UHFFFAOYSA-N 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical group [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 150000001299 aldehydes Chemical class 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000001273 butane Substances 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000008246 gaseous mixture Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical group 0.000 description 1
- 230000000977 initiatory effect Effects 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 1
- 239000004530 micro-emulsion Substances 0.000 description 1
- IJDNQMDRQITEOD-UHFFFAOYSA-N n-butane Chemical compound CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 description 1
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 238000009275 open burning Methods 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000001294 propane Substances 0.000 description 1
- 239000000779 smoke Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 238000000352 supercritical drying Methods 0.000 description 1
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Abstract
The invention discloses a monolithic catalyst for dimethyl ether catalytic combustion and a preparation method and an application thereof; the catalyst adopts cordierite as carrier, organic matter as adhesive and manganese oxide molecular sieve as active component; the monolithic catalyst is prepared by the coating method that the catalyst is stirred in high speed under the action of the organic adhesive to prepare slurry and then the slurry is coated on cordierite. The catalyst of the invention is used for dimethyl ether catalytic combustion and the catalytic combustion of dimethyl ether can be fully completed at 160-335 DEG C and the volume ratio of air or gas mixture to dimethyl ether is 50. The monolithic catalyst has simple process and low cost, thus being a high effective and clean catalyst for dimethyl ether catalytic combustion.
Description
Technical field
The present invention relates to be used for the integral catalyzer and preparation method thereof of a kind of dimethyl ether catalytic combustion of clean energy resource dimethyl ether catalytic combustion.
Background technology
Dimethyl ether (DME) has good combustibility, and is harmless to atmospheric ozone layer, and sulfur-bearing, nitrogen can not produce black smoke during burning, can not produce SO
xWith NO
xFrom the domestic fuel angle, dimethyl ether has and the similar rerum natura of liquefied petroleum gas (LPG), can be used as the substitute of ultra-clean diesel oil and LPG.From the railroad fuel angle analysis: dimethyl ether Cetane number height, power performance is good, has incomparable comprehensive advantages such as natural gas, methyl alcohol, propane, butane, diesel oil.The physical property that dimethyl ether is good, the decline of the production of multi-source and manufacturing cost in addition, making it becomes possibility as clean fuel.
Though DME fuel has high efficiency and oligosaprobic advantage, in the open burning, the dimethyl ether initiation temperature is higher, incomplete combustion, and engine nitrogen oxide, particulate, non-methane is hydrocarbon and emission of harmful substances such as aldehydes pollutes environment.Thereby, adopt the mode of catalytic combustion, can make dimethyl ether under catalyst action under lower temperature deep oxidation, and then cause combustion reaction fast, thereby realization completing combustion, improve the utilization ratio of fuel, realize environmental protection and purpose of energy saving, this is particularly important as power plant fuel, railroad fuel and domestic fuel to it.
The advantage of catalytic combustion is to reduce ignition temperature significantly, realizes clean burning, improves the utilization ratio of fuel.Yu Qian etc. have prepared hexa-aluminate catalyzer in the reverse microemulsion system that Chinese patent (application number 200710030831.3) adopts OP-10, n-octyl alcohol, normal heptane and water to form in conjunction with Supercritical Drying Technology, as Ni
1-xMn
xBaAl
11O
19-δ, LaMAl
11O
19-δ(M=Ni, Cu, Co, Mn, Fe) and MnBaAl
11O
19-δ, be used for the catalytic combustion of dimethyl ether.Find to adopt organic bond to prepare integral catalyzer in addition and be used for the relevant report of dimethyl ether catalytic combustion.
Summary of the invention
The object of the present invention is to provide a kind of integral catalyzer that is used for dimethyl ether catalytic combustion.A kind of preparation method of integral catalyzer of dimethyl ether catalytic combustion and the application in dimethyl ether catalytic combustion thereof also are provided.
The integral catalyzer of a kind of dimethyl ether catalytic combustion provided by the invention adopts cordierite as carrier, is adhesive with the organic matter, is active component with the manganese oxide molecular sieve.
The hole density of above-mentioned cordierite is 20 hole/inches
2～400 hole/inches
2
Above-mentioned manganese oxide molecular sieve has the cryptomelane structure.
Above-mentioned oxygen adhesive is a polyvinyl alcohol, perhaps polyethylene glycol, perhaps methoxy poly (ethylene glycol), perhaps poly-oxireme ether-poly-propylene oxide ether-poly-oxireme ether.
The present invention also provides the preparation method of the integral catalyzer of described dimethyl ether catalytic combustion, has the following steps:
(1) mass percent by adhesive and manganese oxide molecular sieve is 8%～60%, takes by weighing adhesive and manganese oxide molecular sieve, adds proper amount of deionized water, and high-speed stirred 1～8h adds thermal agitation 3～15h again, obtains the manganese oxide molecular sieve slurries;
(2) cordierite carrier is immersed in the above-mentioned manganese oxide molecular sieve slurries, take out the back among dipping 1～60min, blows the raffinate in the most duct, dries in the shade in air, dry 4～24h under 60～120 ℃ of conditions then is warmed up to 350～800 ℃ of roasting 2～6h with the speed of 1.5～4 ℃/min.
The present invention also provides the integral catalyzer of described dimethyl ether catalytic combustion to be applied to the catalytic combustion of dimethyl ether.
Catalyst of the present invention is used for the catalytic combustion of dimethyl ether, is under 50 the condition in the volume ratio of air or gaseous mixture and dimethyl ether, in 160～335 ℃ with the complete catalytic combustion of dimethyl ether.
The invention has the beneficial effects as follows: the dimethyl ether catalytic combustion catalyst that the invention provides a kind of Cheap highly effective cleaning, can reduce the ignition temperature of dimethyl ether, reduce pollutant emission, improve utilization efficiency of energy, especially be adapted to the catalytic combustion of dimethyl ether under the high-speed condition.
In this patent, we have prepared the integral catalyzer of manganese oxide octahedron molecular screen (OMS-2), and with it catalyst combustion reaction that is applied to the clean energy resource dimethyl ether, have realized the clean burning of efficient cryogenic, and product has only carbon dioxide and water.
Description of drawings
Fig. 1 is the characteristic X-ray diffraction pattern (XRD) of blank cordierite (a) and OMS-2/ cordierite catalyst (b).
Fig. 2 is the conversion ratio and the temperature relation figure of dimethyl ether catalytic combustion on the OMS-2/ cordierite catalyst.
The specific embodiment
Embodiment 1: by the polyvinyl alcohol and the mass percent of manganese oxide molecular sieve is that 27.83% proportioning is mixed, and adds the deionized water of 30ml, and high-speed stirred 1h adds thermal agitation 3h again, obtains the manganese oxide molecular sieve slurries.With the hole density of anticipating is 400 hole/inches
2Honeycomb ceramic carrier be immersed in the manganese oxide molecular sieve slurries that prepare, take out the back among the dipping 30min, blows the raffinate in the most duct, and back 80 ℃ of dry 12h dry in the shade in air, speed with 1.5 ℃/min is raised to 450 degree roasting 2h, obtains manganese oxide molecular sieve honeycomb ceramic integral formula catalyst.
Embodiment 2: by the polyvinyl alcohol and the mass percent of manganese oxide molecular sieve is that 27.83% proportioning is mixed, and adds the deionized water of 30ml, and high-speed stirred 4h adds thermal agitation 15h again, obtains the manganese oxide molecular sieve slurries.With the hole density of anticipating is 400 hole/inches
2Honeycomb ceramic carrier be immersed in the manganese oxide molecular sieve slurries that prepare, take out the back among the dipping 30min, blows the raffinate in the most duct, and back 80 ℃ of dry 12h dry in the shade in air, speed with 1.5 ℃/min is raised to 450 degree roasting 2h, obtains manganese oxide molecular sieve honeycomb ceramic integral formula catalyst.
Embodiment 3: by the polyethylene glycol and the mass percent of manganese oxide molecular sieve is that 8% proportioning is mixed, and adds the deionized water of 30ml, and high-speed stirred 8h adds thermal agitation 3h again, obtains the manganese oxide molecular sieve slurries.With the hole density of anticipating is 400 hole/inches
2Honeycomb ceramic carrier be immersed in the manganese oxide molecular sieve slurries that prepare, take out the back among the dipping 60min, blows the raffinate in the most duct, and back 80 ℃ of dry 12h dry in the shade in air, speed with 1.5 ℃/min is raised to 450 degree roasting 2h, obtains manganese oxide molecular sieve honeycomb ceramic integral formula catalyst.
Embodiment 4: by the polyethylene glycol and the mass percent of manganese oxide molecular sieve is that 60% proportioning is mixed, and adds the deionized water of 60ml, and high-speed stirred 8h adds thermal agitation 3h again, obtains the manganese oxide molecular sieve slurries.With the hole density of anticipating is 400 hole/inches
2Honeycomb ceramic carrier be immersed in the manganese oxide molecular sieve slurries that prepare, take out the back among the dipping 60min, blows the raffinate in the most duct, and back 60 ℃ of dry 24h dry in the shade in air, speed with 4 ℃/min is raised to 450 degree roasting 2h, obtains manganese oxide molecular sieve honeycomb ceramic integral formula catalyst.
Embodiment 5: by the methoxy poly (ethylene glycol) and the mass percent of manganese oxide molecular sieve is that 27.83% proportioning is mixed, and adds the deionized water of 60ml, and high-speed stirred 8h adds thermal agitation 8h again, obtains the manganese oxide molecular sieve slurries.With the hole density of anticipating is 400 hole/inches
2Honeycomb ceramic carrier be immersed in the manganese oxide molecular sieve slurries that prepare, take out the back among the dipping 30min, blows the raffinate in the most duct, and back 80 ℃ of dry 12h dry in the shade in air, speed with 1.5 ℃/min is raised to 450 degree roasting 2h, obtains manganese oxide molecular sieve honeycomb ceramic integral formula catalyst.
Embodiment 6: by the methoxy poly (ethylene glycol) and the mass percent of manganese oxide molecular sieve is that 27.83% proportioning is mixed, and adds the deionized water of 45ml, and high-speed stirred 8h adds thermal agitation 3h again, obtains the manganese oxide molecular sieve slurries.With the hole density of anticipating is 200 hole/inches
2Honeycomb ceramic carrier be immersed in the manganese oxide molecular sieve slurries that prepare, take out the back among the dipping 30min, blows the raffinate in the most duct, and back 80 ℃ of dry 12h dry in the shade in air, speed with 1.5 ℃/min is raised to 450 degree roasting 4h, obtains manganese oxide molecular sieve honeycomb ceramic integral formula catalyst.
Embodiment 7: by the methoxy poly (ethylene glycol) and the mass percent of manganese oxide molecular sieve is that 8% proportioning is mixed, and adds the deionized water of 60ml, and high-speed stirred 1h adds thermal agitation 3h again, obtains the manganese oxide molecular sieve slurries.With the hole density of anticipating is 400 hole/inches
2Honeycomb ceramic carrier be immersed in the manganese oxide molecular sieve slurries that prepare, take out the back among the dipping 5min, blows the raffinate in the most duct, and back 80 ℃ of dry 12h dry in the shade in air, speed with 4 ℃/min is raised to 800 degree roasting 2h, obtains manganese oxide molecular sieve honeycomb ceramic integral formula catalyst.
Embodiment 8: by the poly-oxireme ether-poly-propylene oxide ether-poly-oxireme ether and the mass percent of manganese oxide molecular sieve is that 27.83% proportioning is mixed, the deionized water that adds 60ml, high-speed stirred 1h adds thermal agitation 3h again, obtains the manganese oxide molecular sieve slurries.With the hole density of anticipating is 20 hole/inches
2Honeycomb ceramic carrier be immersed in the manganese oxide molecular sieve slurries that prepare, take out the back among the dipping 1min, blows the raffinate in the most duct, and back 120 ℃ of dry 4h dry in the shade in air, speed with 3 ℃/min is raised to 350 degree roasting 6h, obtains manganese oxide molecular sieve honeycomb ceramic integral formula catalyst.
Claims (5)
1. the integral catalyzer of a dimethyl ether catalytic combustion, it is characterized in that this catalyst adopts cordierite as carrier, with polyvinyl alcohol or polyethylene glycol or methoxy poly (ethylene glycol) or poly-oxireme ether-poly-propylene oxide ether-poly-oxireme ether is adhesive, is active component with manganese oxide molecular sieve OMS-2; The mass percent of above-mentioned adhesive and manganese oxide molecular sieve OMS-2 is 8%～60%.
2. the integral catalyzer of dimethyl ether catalytic combustion according to claim 1, the hole density that it is characterized in that above-mentioned cordierite is 20 hole/inches
2～400 hole/inches
2
3. the integral catalyzer of dimethyl ether catalytic combustion according to claim 1 is characterized in that above-mentioned manganese oxide molecular sieve has the cryptomelane structure.
4. the preparation method of the integral catalyzer of dimethyl ether catalytic combustion described in the claim 1 is characterized in that having the following steps:
(1) be 8%～60% to take by weighing adhesive and manganese oxide molecular sieve OMS-2 by the mass percent of adhesive and manganese oxide molecular sieve OMS-2, add proper amount of deionized water, high-speed stirred 1～8h adds thermal agitation 3～15h again, obtains the manganese oxide molecular sieve slurries;
(2) cordierite carrier is immersed in the above-mentioned manganese oxide molecular sieve slurries, take out the back among dipping 1～60min, blows the raffinate in the most duct, dries in the shade in air, dry 4～24h under 60～120 ℃ of conditions then is warmed up to 350～800 ℃ of roasting 2～6h with the speed of 1.5～4 ℃/min.
5. the integral catalyzer of dimethyl ether catalytic combustion described in the claim 1 is applied to the catalytic combustion of dimethyl ether.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2009100417998A CN101628241B (en) | 2009-08-11 | 2009-08-11 | Monolithic catalyst for dimethyl ether catalytic combustion and preparation method and application thereof |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2009100417998A CN101628241B (en) | 2009-08-11 | 2009-08-11 | Monolithic catalyst for dimethyl ether catalytic combustion and preparation method and application thereof |
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| CN101628241A CN101628241A (en) | 2010-01-20 |
| CN101628241B true CN101628241B (en) | 2011-11-09 |
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| CN102921454B (en) * | 2012-06-28 | 2015-07-22 | 北京化工大学 | Preparation method of monolithic BEA molecular sieve catalyst for direct N2O catalysis decomposition |
| CN103111322A (en) * | 2013-02-03 | 2013-05-22 | 北京化工大学 | Preparation method of integral cellular molecular sieve based catalyst for N2O decomposition |
| CN109830694B (en) * | 2019-01-25 | 2021-03-02 | 宁波石墨烯创新中心有限公司 | Catalyst with double-coating structure and preparation method and application thereof |
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