CN1676199A - Nano-molecular sieve materials as catalysts for the reduction of acetylene to eliminate NOx in aerobic exhaust gas - Google Patents
Nano-molecular sieve materials as catalysts for the reduction of acetylene to eliminate NOx in aerobic exhaust gas Download PDFInfo
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- CN1676199A CN1676199A CN 200410010546 CN200410010546A CN1676199A CN 1676199 A CN1676199 A CN 1676199A CN 200410010546 CN200410010546 CN 200410010546 CN 200410010546 A CN200410010546 A CN 200410010546A CN 1676199 A CN1676199 A CN 1676199A
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- molecular sieve
- zeolite
- catalyst
- nano
- acetylene
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- 239000003054 catalyst Substances 0.000 title claims abstract description 54
- 239000002808 molecular sieve Substances 0.000 title claims abstract description 45
- 239000000463 material Substances 0.000 title claims abstract description 37
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 title claims abstract description 30
- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 title claims abstract description 30
- 230000009467 reduction Effects 0.000 title claims description 12
- 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 32
- 239000010457 zeolite Substances 0.000 claims description 25
- 229910021536 Zeolite Inorganic materials 0.000 claims description 24
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 24
- 239000000203 mixture Substances 0.000 claims description 12
- 241000269350 Anura Species 0.000 claims description 5
- 239000011248 coating agent Substances 0.000 claims description 5
- 238000000576 coating method Methods 0.000 claims description 5
- 238000003379 elimination reaction Methods 0.000 claims description 5
- 238000002360 preparation method Methods 0.000 claims description 5
- 239000007787 solid Substances 0.000 claims description 5
- 230000008030 elimination Effects 0.000 claims description 3
- 239000002994 raw material Substances 0.000 claims 3
- JYIMWRSJCRRYNK-UHFFFAOYSA-N dialuminum;disodium;oxygen(2-);silicon(4+);hydrate Chemical compound O.[O-2].[O-2].[O-2].[O-2].[O-2].[O-2].[Na+].[Na+].[Al+3].[Al+3].[Si+4] JYIMWRSJCRRYNK-UHFFFAOYSA-N 0.000 claims 1
- 239000007789 gas Substances 0.000 abstract description 27
- 239000003638 chemical reducing agent Substances 0.000 abstract description 14
- 239000002912 waste gas Substances 0.000 abstract description 10
- 238000002485 combustion reaction Methods 0.000 abstract description 7
- 239000002440 industrial waste Substances 0.000 abstract description 7
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 abstract description 6
- 238000000034 method Methods 0.000 abstract description 2
- 238000006243 chemical reaction Methods 0.000 description 10
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 8
- 231100000331 toxic Toxicity 0.000 description 8
- 230000002588 toxic effect Effects 0.000 description 8
- 241000264877 Hippospongia communis Species 0.000 description 7
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 6
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- 239000000919 ceramic Substances 0.000 description 6
- 239000011230 binding agent Substances 0.000 description 5
- 238000001354 calcination Methods 0.000 description 5
- 239000002245 particle Substances 0.000 description 5
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 4
- 229910021529 ammonia Inorganic materials 0.000 description 4
- 238000005259 measurement Methods 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 description 4
- 238000006722 reduction reaction Methods 0.000 description 4
- 229910001593 boehmite Inorganic materials 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 239000002131 composite material Substances 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 3
- 150000002500 ions Chemical class 0.000 description 3
- 239000003595 mist Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 2
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 2
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical class CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 description 2
- 229910004298 SiO 2 Inorganic materials 0.000 description 2
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 2
- 229910052787 antimony Inorganic materials 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 239000004202 carbamide Substances 0.000 description 2
- 238000010531 catalytic reduction reaction Methods 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 229910052733 gallium Inorganic materials 0.000 description 2
- 229910052732 germanium Inorganic materials 0.000 description 2
- 229910052738 indium Inorganic materials 0.000 description 2
- 238000005342 ion exchange Methods 0.000 description 2
- 239000001294 propane Substances 0.000 description 2
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 2
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 2
- 229910052761 rare earth metal Inorganic materials 0.000 description 2
- 229910052709 silver Inorganic materials 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 229910052718 tin Inorganic materials 0.000 description 2
- 229910052727 yttrium Inorganic materials 0.000 description 2
- 229910052726 zirconium Inorganic materials 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 241001012508 Carpiodes cyprinus Species 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- 229910003077 Ti−O Inorganic materials 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 238000002513 implantation Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 239000000618 nitrogen fertilizer Substances 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 238000004088 simulation Methods 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
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- Catalysts (AREA)
Abstract
The present invention relates to a nano molecular sieve material catalyst which uses acetylene mixed gas as reducing agent and can be used for reducing and eliminating nitrogen oxide (Nox) in aerobic waste gas. Said invention is characterized by that the application range of said molecular sieve material catalyst is that using acetylene or acetylene mixed gas as reducing agent to catalyze, reduce and eliminate Nox in tail gas of internal combustion engine and diesel engine and Nox in the aerobic industrial waste gas. Besides, said invention also provides the application method of said catalyst.
Description
Technical field
The invention belongs to the atmosphere environmental technology field, relate to the nano molecular sieve material, specially refer to that to be used for acetylene or acetylene gas mixture be the NO that the reducing agent catalytic reduction is eliminated aerobic waste gas
x
Background technology
In many factories, in factory's exhaust gas discharged such as steam power plant, nitric acid manufactory, nitrogen fertilizer plant, and the NO that all contains variable concentrations in the tail gas of internal combustion engine, diesel emission
xNO
xTo health is very harmful, so countries in the world are to the NO in various stationary source toxic emissions (toxic emission of factory) and the various moving source toxic emission (engine discharging tail gas)
xContent has all been worked out strict rules and has been limited.
NO in the aerobic toxic emission source
xEliminate, employed catalyst is different because of the difference of reducing agent.Even because eliminate identical NO in the same emission source
x, the reducing agent difference has also caused different reactions and has eliminated mechanism.As, application Cu-Cr-O catalyst or W-V-Ti-O catalyst are applied to the NO in the stationary source toxic emission earlier when being reducing agent with ammonia or urea
xEliminate.And use methane, ethane, propane, C at present
4Alkane, C
6Alkane, C
8Alkane, C
12Alkane and ethene, these lower carbon number hydrocarbons of propylene, or low-carbon alcohols such as methyl alcohol, ethanol, propyl alcohol, butanols is reducing agent, and it is varied that the catalyst that is used to study then has, as Ag/Al
2O
3, Ga/Al
2O
3, Cu-ZSM-5, Co-ZSM-5, Ga/MOR, Ge-H-BEA, Ce-H-FER etc.For NO in the aerobic toxic emission source
xEliminate reaction, be studied and report, owing to acetylene or acetylene mixture do not have human NO in aerobic toxic emission source as yet so far though have multiple molecular sieve catalysts
xEliminate reaction, so the application of corresponding catalyst and research report belong to blank at present.
For NO in the aerobic toxic emission source
xEliminate reaction, no matter technology in the past and research are at solving NO
xNO in the fixed discharge source
xElimination or NO
xNO in the mobile emission source
xElimination all exist and much be difficult to the shortcoming that overcomes.Eliminate NO in the aerobic waste gas with ammonia or urea as reducing agent
xShi Rongyi causes the secondary pollution of ammonia.With methane, ethane, propane, C
4Alkane, C
6Alkane, C
8Alkane, C
12Alkane is reducing agent or is reducing agent with ethene, propylene, or is that reducing agent is eliminated NO in the aerobic waste gas with low-carbon (LC)s such as methyl alcohol, ethanol, propyl alcohol, butanols
xReaction, the selective reaction result who does not find appropriate catalyst to obtain as yet to have application value.And be that reducing agent is eliminated NO in the aerobic waste gas with acetylene or acetylene mixture
xReaction, the someone carries out catalyticing research as yet.
Summary of the invention
The purpose of this invention is to provide a kind of average particle crystalline substance and be the nano molecular sieve material catalyst of 5nm～500nm, being used for acetylene or acetylene gas mixture is that aerobic nitrogen oxides from exhaust gas (NO is eliminated in the reducing agent reduction
x), comprise NO in the catalytic reduction elimination aerobic industrial waste gas
xWith the NO in internal combustion engine, the diesel engine tail gas
x
Technical scheme of the present invention is as follows:
Related nano molecular sieve material catalyst of the present invention can be made granular pattern and two kinds of forms of monolithic devices in use.Granular pattern nano molecular sieve material catalyst is that following grain crystalline substance is joined a micron molecular sieve, Al for the molecular sieve of nanoscale
2O
3, CeO
2, SiO
2, or other inorganic binder in to make the mass fraction of following nano molecular sieve material in catalyst be 10～100%, make particle or extrusion obtains.Monolithic devices nano molecular sieve material catalyst is to add 0～90% micron molecular sieve, Al in following nano molecular sieve material
2O
3, CeO
2, SiO
2, or other inorganic binder after on ceramic honey comb or metal support, make coating, making the mass fraction of following nano molecular sieve material in the solids of coating is 10～100%, or it directly is squeezed into honeycomb type (no supporter), making the mass fraction of following nano molecular sieve material in monolithic devices nano molecular sieve material catalyst is 10～100% to make and obtain.
One of the nano molecular sieve ZSM-5 zeolite that it is 5nm～500nm that the related nano molecular sieve material of above-mentioned granular pattern and monolithic devices nano molecular sieve material catalyst is meant by the brilliant diameter of grain, SAPO zeolite, FER zeolite, β zeolite, A type zeolite set out, or set out by the mixture that two or more above-mentioned nano molecular sieve zeolites are wherein formed, resulting A, B, C, the D four kinds of elements sieve material:
Category-A. the molecular screen material of Hydrogen or ammonia type or their composite material.
Category-B. one of rare earth element, Y, Sn, Ge, Sb, Zr, Ti, Bi, Ag, In, Ga ion, or wherein two kinds of ions or the molecular screen material of different kinds of ions exchange or their composite material.
The C class. with one of rare earth element, precious metal element, Y, Sn, Ge, Sb, Zr, Ti, Bi, Ag, In, Ga, or wherein two kinds of elements or multiple element are supported on the molecular screen material that obtains on above-mentioned A group material, B group material or its composite material.
The mixture of D class .A, B, three kinds of molecular screen materials of C or wherein any two kinds mixture.
The using method of nano molecular sieve material catalyst of the present invention is, to containing NO
xThe aerobic industrial waste gas or internal combustion engine, diesel engine tail gas in inject acetylene or acetylene gas mixture (acetylene is 10%～100% in the concentration of mist) makes acetylene after the concentration of waste gas reaches 10～4000ppm, mist is imported temperature be controlled in the molecular sieve catalyst involved in the present invention in 200～500 ℃ of scopes, make the NO in aerobic industrial waste gas or internal combustion engine, the diesel engine tail gas thus
xEliminate with the acetylene reduction.The implantation concentration of acetylene in waste gas can be according to NO in the waste gas
xConcentration suitably control, its reference volume concentration is the NO in aerobic industrial waste gas or the engine discharging tail gas
x1/4～1 times of concentration of treatment.
Effect of the present invention and benefit are that this nano molecular sieve material is used for the acetylene reduction as catalyst and eliminates aerobic industrial waste gas NO
xOr the NO in the internal combustion engine, diesel engine tail gas
xHave than high selectivity, advantages of high catalytic activity and better low temperature activity.
The specific embodiment
Test two-part embodiment by Preparation of Catalyst and catalyst performance below and be described in detail the specific embodiment of the present invention.
Preparation of Catalyst embodiment:
Embodiment 1
10 gram average particle crystalline substances are poured at the Na-ZSM5 of 40nm-80nm molecular sieve be dissolved with 8 gram NH
4NO
3The 50ml aqueous solution in, carried out ion-exchange 10 hours 80 ℃ of stirrings, 120 ℃ of oven dry, after 500 ℃ of calcinings, same again repeated exchanged is handled and is once obtained nanometer H-ZSM-5 (a kind of nano molecular sieve materials A class).
Embodiment 2
Get 4 grams by embodiment 1 gained nanometer H-ZSM5 molecular sieve, pour into and be dissolved with 2mmol Ce (NO
3)
3The 50ml aqueous solution in, carried out ion-exchange 10 hours 80 ℃ of stirrings, 120 ℃ of oven dry obtain nano Ce-H-ZSM-5 (a kind of nano molecular sieve material B class) after 500 ℃ of calcinings.
Embodiment 3
Add 0.5 gram boehmite colloidal binder in by embodiment 1 gained nanometer H-ZSM-5 to 4 grams and be mixed evenly, make particle, oven dry, 500 ℃ of calcinings obtain a kind of nanometer H-ZSM-5 granular pattern catalyst.
Embodiment 4
Add 0.5 gram boehmite colloidal binder in by embodiment 2 gained nano Ce-H-ZSM-5 catalyst to 4 grams and be mixed evenly, make particle, oven dry, 500 ℃ of calcinings obtain a kind of nano Ce-H-ZSM-5 granular pattern catalyst.
Embodiment 5
After in 4 restrain by embodiment 2 gained nano Ce-H-ZSM-5, adding 0.5 gram boehmite colloidal binder and distilled water, twice coated and dried on ceramic honey comb, 500 ℃ of calcinings obtain a kind of nano Ce-H-ZSM-5/ honeycomb ceramic integral type catalyst.Weighing records in this nano Ce-H-ZSM-5/ honeycomb ceramic integral type catalyst, and the shared mass fraction of nano Ce-H-ZSM-5 is about 10%.
Acetylene is that reducing agent is eliminated NO on the catalyst
xEmbodiment:
Embodiment 6
The 20-40 order pack in the fixed bed reactors into by embodiment 3 gained granular pattern nanometer H-ZSM-5 catalyst 200mg, and feeding overall flow rate under assigned temperature is 50ml/min, and NO concentration is 1600ppm, O
2Concentration is 9.95% and (simulates with this and contain NO
xAerobic industrial waste gas or internal combustion engine, diesel engine tail gas), concentration of acetylene is 800ppm, He is the mist of balance gas.Eliminate NO
xMeasurement result list in the table 1.
Embodiment 7
Use by embodiment 4 gained granular pattern nano Ces-H-ZSM-5 granular pattern catalyst and replace among the embodiment 6 eliminating NO by embodiment 3 gained granular pattern nanometer H-ZSM-5 catalyst
xMeasurement result list in the table 1.
Embodiment 8
Get a part (25mm * φ 15mm) by embodiment 5 gained nano Ce-H-ZSM-5/ honeycomb ceramic integral type catalyst, be fixed in the supporting with it quartz tube reactor, allow the reacting gas that enters reaction tube this catalyst of all flowing through with embodiment 6 identical proportionings.Change total gas couette, just make the acetylene in the reacting gas under 350 ℃, transform corresponding elimination NO fully
xMeasurement result list in the table 1.
Table 1. simulation is containing NO
xAerobic waste gas in eliminate NO
xMeasurement result
| Catalyst | Reaction temperature/℃ | ?NO xConversion ratio (generates N 2)％ | |
| Embodiment 6 | Nanometer H-ZSM-5 granular pattern catalyst | ???325 | ????80 |
| Embodiment 7 | Nano Ce-H-ZSM-5 granular pattern catalyst | ???325 | ????95 |
| Embodiment 8 | Nano Ce-H-ZSM-5/ honeycomb ceramic integral catalyzer | ???350 | ????86 |
Claims (4)
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 200410010546 CN1676199A (en) | 2004-12-30 | 2004-12-30 | Nano-molecular sieve materials as catalysts for the reduction of acetylene to eliminate NOx in aerobic exhaust gas |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 200410010546 CN1676199A (en) | 2004-12-30 | 2004-12-30 | Nano-molecular sieve materials as catalysts for the reduction of acetylene to eliminate NOx in aerobic exhaust gas |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN1676199A true CN1676199A (en) | 2005-10-05 |
Family
ID=35049037
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|---|---|---|---|
| CN 200410010546 Pending CN1676199A (en) | 2004-12-30 | 2004-12-30 | Nano-molecular sieve materials as catalysts for the reduction of acetylene to eliminate NOx in aerobic exhaust gas |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101468295B (en) * | 2007-12-28 | 2011-08-10 | 中国石油大学(北京) | Combined catalyst for simultaneously eliminating four kinds of pollutants from diesel exhaust and purification method |
| CN102513150A (en) * | 2011-11-14 | 2012-06-27 | 天津大学 | SAPO (Silicoaluminophosphate) molecular sieve SCR (Selective Catalytic Reduction) catalyst, preparation thereof and application thereof in removal of acrylonitrile tail gas NOx |
| CN101711991B (en) * | 2009-10-15 | 2012-07-18 | 清华大学 | Fe molecular sieve composite catalyst and preparation method thereof |
| CN106413888A (en) * | 2014-02-07 | 2017-02-15 | 日立造船株式会社 | Catalyst for purifying combustion exhaust gas and method for purifying combustion exhaust gas |
| CN112275138A (en) * | 2020-10-15 | 2021-01-29 | 清华大学 | Preparation method of denitration synergistic additive for circulating fluidized bed boiler |
-
2004
- 2004-12-30 CN CN 200410010546 patent/CN1676199A/en active Pending
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101468295B (en) * | 2007-12-28 | 2011-08-10 | 中国石油大学(北京) | Combined catalyst for simultaneously eliminating four kinds of pollutants from diesel exhaust and purification method |
| CN101711991B (en) * | 2009-10-15 | 2012-07-18 | 清华大学 | Fe molecular sieve composite catalyst and preparation method thereof |
| CN102513150A (en) * | 2011-11-14 | 2012-06-27 | 天津大学 | SAPO (Silicoaluminophosphate) molecular sieve SCR (Selective Catalytic Reduction) catalyst, preparation thereof and application thereof in removal of acrylonitrile tail gas NOx |
| CN106413888A (en) * | 2014-02-07 | 2017-02-15 | 日立造船株式会社 | Catalyst for purifying combustion exhaust gas and method for purifying combustion exhaust gas |
| JPWO2015119069A1 (en) * | 2014-02-07 | 2017-03-23 | 日立造船株式会社 | Combustion exhaust gas purification catalyst and combustion exhaust gas purification method |
| CN112275138A (en) * | 2020-10-15 | 2021-01-29 | 清华大学 | Preparation method of denitration synergistic additive for circulating fluidized bed boiler |
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