CN105148933A - Denitration catalyst for glass kiln and preparation method of denitration catalyst - Google Patents
Denitration catalyst for glass kiln and preparation method of denitration catalyst Download PDFInfo
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- CN105148933A CN105148933A CN201510515083.2A CN201510515083A CN105148933A CN 105148933 A CN105148933 A CN 105148933A CN 201510515083 A CN201510515083 A CN 201510515083A CN 105148933 A CN105148933 A CN 105148933A
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Abstract
The invention discloses a denitration catalyst for a glass kiln and a preparation method of the denitration catalyst. The performance of the catalyst is improved by adding iron and rare earth elements, so that the catalyst adapts to the smoke condition of the glass kiln, and the best denitration effect is achieved. The provided catalyst can increase the width of a window reflecting the temperature and suitable for being used at the temperature interval of 240 DEG C-430 DEG C, the sulfur conversion rate is reduced, the denitration efficiency is improved, and the preparation method can be applicable to production of cellular denitration catalysts and plate-type denitration catalysts.
Description
Technical field
The invention belongs to denitrating flue gas processing technology field, relate to a kind of glass furnace denitrating catalyst and preparation method thereof.
Background technology
At present, the denitration technology of commercial Application is mainly divided into low NOx combusting technology, SNCR technology and SCR technology in the world.SCR (SCR) denitration technology has high NOx extrusion rate, be at present application at most, the most ripe gas denitrifying technology, this technology utilizes NH having under catalyst existent condition
3deng reducing agent, NOx is reduced into N
2and H
2o, thus reach NO_x removal, the object of pollution abatement.
Along with the reinforcement of Environmental protection, each fume emission industry is proposed to the requirement of smoke gas treatment, in recent years, along with the concern of government, glass furnace tail gas denitration process is made enterprise by each glass and puts on transformation schedule.What current most of glass furnace was installed is import cellular catalyst, and cost is high, mainly due to Gas Parameters that glass furnace is special.The main feature of glass furnace fume: flue-gas temperature is high, flue gas flow is moderate, SO in flue gas
2content content that is higher, dust lower.
The technology of domestic current employing is mainly conventional vanadium tungsten titanium system and vanadium molybdenum titanium system, and this technology is mainly administered for the denitration of coal-fired plant flue gas, the main feature of coal-fired plant flue gas: flue-gas temperature is moderate, flue gas flow is large, SO in flue gas
2content lower, the content of dust is high.Although be reach denitration process equally, the heterogeneity of two kinds of flue gases determines that the denitration efficiency of catalyst and O&M require different.
Summary of the invention
For meeting the higher denitration efficiency of glass furnace Combustion in High Temperature High Sulfur flue gas and lower sulphur conversion ratio, the present invention proposes a kind of glass furnace denitrating catalyst and preparation method thereof, by adding iron and rare earth element, improve catalyst performance, thus adapt to glass furnace fume condition, reach best denitration effect.
The concrete technical scheme for above-mentioned technical problem is as follows:
A kind of glass furnace denitrating catalyst, by weight, comprising:
TiO
250-60 part,
Ammonium metavanadate 0.5-2 part,
Ammonium heptamolybdate or ammonium paratungstate 2-5 part,
Ammoniacal liquor 1-2 part,
Deionized water 25-30 part,
Source of iron 1-5 part,
Cerium source 0.5-3 part,
Other additives 5-10 part, other additives are selected from the combination of potter's clay, glass and CMC, or the combination of potter's clay, glass and paper fibre, or the combination of potter's clay, glass, paper fibre and CMC.
The mass concentration (g/mL) of above-mentioned ammoniacal liquor is 0.091-0.227g/ml, preferred 0.227g/ml.
Above-mentioned source of iron can be the ferrous oxide, ferric nitrate etc. of iron oxide, the not sulfur-bearing of not sulfur-bearing, preferably the iron oxide of not sulfur-bearing;
Above-mentioned cerium source can be cerous nitrate, cerium oxide etc., preferential oxidation cerium.
Further, the preferred TiO of the composition of above-mentioned catalyst
260 parts, ammonium metavanadate 2 parts, ammonium heptamolybdate or ammonium paratungstate 5 parts, ammoniacal liquor 2 parts, deionized water 30 parts, iron oxide 2 parts, cerium oxide 1 part, 4 parts, potter's clay, glass 2 parts, CMC1 part.
A second aspect of the present invention provides a kind of preparation method of glass furnace denitrating catalyst, and concrete steps are as follows:
1) by TiO
2, ammonium heptamolybdate or ammonium paratungstate add a part of deionized water after being dry mixed 5-10min, stir 10-20min;
2) add ammonium metavanadate, stir 10-20min;
3) add ammoniacal liquor when adding source of iron and cerium source simultaneously, stir 20-30min; Add other additives, stir 10-20min;
4) add residue deionized water, reverse agitating function mixes, and hydrofuge, obtains mixture pug.
Above-mentioned steps 1) in by TiO
2, ammonium heptamolybdate or ammonium paratungstate drop in mixing roll or kneader and are dry mixed.
Above-mentioned steps 1), 2) and 3) in mixing speed 450-750 rev/min, preferably 500 revs/min.
Above-mentioned steps 3) in, the addition sequence of source of iron and cerium source and other additives is not fixed.
Above-mentioned mixture pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.
Said method also comprises: use extruder or coating line to make honeycomb type denitrification catalyst or plate-type denitration catalyst mixture pug, and at 520-560 degree calcining 4-8 hour, preferably 550 degree of calcinings 6 hours.
Technique effect of the present invention is as follows:
Catalyst provided by the invention can increase reflection temperature window width, is applicable to 240-430 degree temperature range, reduces sulphur conversion ratio, improve denitration efficiency, go for the production of honeycomb type denitrification catalyst and plate-type denitration catalyst.
Accompanying drawing explanation
Fig. 1 is the embodiment of the present invention 2 and comparative example denitration efficiency comparison diagram at different temperatures.
Detailed description of the invention
Embodiment 1
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Add 2 parts of ammoniacal liquor when adding 0.5 part of cerium oxide, 500 revs/min are stirred 20-30min simultaneously; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of CMC, 500 revs/min are stirred 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
Embodiment 2
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Add 2 parts of ammoniacal liquor when adding 1 part of cerium oxide, 500 revs/min are stirred 20-30min simultaneously; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of CMC, stir 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
Embodiment 3
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Add 2 parts of ammoniacal liquor when adding 3 parts of cerium oxide, 500 revs/min are stirred 20-30min simultaneously; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of paper fibre, 500 revs/min are stirred 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
Embodiment 4
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Add 2 parts of ammoniacal liquor when adding 1 part of iron oxide, 500 revs/min are stirred 20-30min simultaneously; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of CMC, 500 revs/min are stirred 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
Embodiment 5
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Add 2 parts of ammoniacal liquor when adding 2 parts of iron oxide, 500 revs/min are stirred 20-30min simultaneously; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of paper fibre, 1 part of CMC, 500 revs/min are stirred 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
Embodiment 6
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Add 2 parts of ammoniacal liquor when adding 5 parts of iron oxide, 500 revs/min are stirred 20-30min simultaneously; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of CMC, 500 revs/min are stirred 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
Embodiment 7
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Add ammoniacal liquor when adding iron oxide 2 parts and 1 part of cerium oxide, 500 revs/min are stirred 20-30min simultaneously; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of CMC, 500 revs/min are stirred 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
Embodiment 8
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Add 2 parts of ammoniacal liquor when adding ferrous oxide 2 parts and 1.5 parts of cerium oxide, 500 revs/min are stirred 20-30min simultaneously; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of CMC, 500 revs/min are stirred 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
Embodiment 9
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Add 2 parts of ammoniacal liquor when adding ferric nitrate 6 parts and 1.5 parts of cerous nitrates, 500 revs/min are stirred 20-30min simultaneously; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of CMC, 500 revs/min are stirred 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
Comparative example
By 60 parts of TiO
2, 5 parts of ammonium heptamolybdates drop into mixing roll or kneader, add 20 parts of deionized waters after being dry mixed 5-10min, and 500 revs/min are stirred 10-20min; Add 2 parts of ammonium metavanadates, 500 revs/min are stirred 10-20min; Continue 500 revs/min and stir 20-30min; Add 4 parts of potter's clay, 2 parts of glasses, 1 part of CMC, 500 revs/min are stirred 10-20min; Add residue 10 parts of deionized waters, with 350 revs/min of speed reverse agitating function mixings, hydrofuge, obtains mixture pug, and described pug moisture 27-31% ± 1%, pH scope is 8.5 ± 0.5.Mixture pug uses extruder to make honeycomb type denitrification catalyst, 550 degree of calcinings 6 hours.
The catalyst prod utilizing above-described embodiment to make detects specific area, wearing and tearing, and configure component and the following simulated flue gas of concentration: CNOx=CNH3=0.045%, CHg=40 μ g/L, CO2 ≈ 4.8%, CH2O ≈ 6.0%, CSO2 ≈ 0.15%, CCO2 ≈ 12%, CHCl ≈ 0.002%, N
2and O
2as Balance Air, air speed GHSV20000m3/h, other components and actual flue gas form basically identical.
Under different flue-gas temperature, the above-mentioned condition of simulated flue gas parameter reference, catalyst denitration efficiency data are as following table:
| Temperature/degree | 240 | 320 | 370 | 400 | 430 |
| Comparative example | 82 | 88 | 91 | 75 | 63 |
| Embodiment 2 | 85 | 90 | 93 | 91 | 87 |
Composition graphs 1 can be found out, adds the catalyst denitration efficiency behind source of iron and cerium source in high-temperature region apparently higher than the denitration efficiency not adding source of iron and cerium source catalyst.
Denitration efficiency and sulphur conversion ratio is measured under 400 degree of simulated flue gas parameters.Data see table
| Specific area (m 3/g) | Denitration efficiency % | Sulphur conversion ratio | |
| Embodiment 1 | 82.06 | 82 | 1.6 |
| Embodiment 2 | 81.61 | 91 | 1.6 |
| Embodiment 3 | 81.45 | 89 | 1.6 |
| Embodiment 4 | 81.80 | 77 | 1.3 |
| Embodiment 5 | 80.23 | 76 | 0.8 |
| Embodiment 6 | 78.93 | 76 | 0.6 |
| Embodiment 7 | 81.11 | 91 | 0.8 |
| Embodiment 8 | 80.90 | 90 | 0.8 |
| Embodiment 9 | 80.72 | 91 | 0.8 |
| Comparative example | 81.78 | 75 | 1.8 |
Can find out in above-described embodiment, interpolation iron oxide and cerium oxide obviously can change catalyst performance, it is made more to adapt to the denitrating flue gas process of Combustion in High Temperature High Sulfur environment, wherein iron oxide add specific area and the sulphur conversion ratio that membership affects catalyst, along with the increase specific area of iron oxide declines slightly, sulphur conversion ratio declines, and down ratio reaches 27.7%-66.7%; The membership that adds of cerium oxide affects denitration efficiency, early stage increases with addition class direct ratio, increase ratio 7%-21%, reaches increment after addition is more than 2 parts not obvious, adds the catalyst denitration efficiency of cerium oxide apparently higher than the typical catalyst not adding cerium oxide.
Therefore optimum proportioning is TiO
260 parts, ammonium metavanadate 2 parts, ammonium heptamolybdate or ammonium paratungstate 5 parts, ammoniacal liquor 2 parts, deionized water 30 parts, iron oxide 2 parts, cerium oxide 1 part, 4 parts, potter's clay, glass 2 parts, CMC1 part.
It should be noted that, the present invention is relative to prior art, key improves catalyst performance by interpolation iron and rare earth element, ammonium heptamolybdate in formula can substitute with ammonium paratungstate, mixing speed during preparation, calcining heat can fluctuate in proper range, or makes plate-type denitration catalyst etc. by coating line, all can not produce material impact to the effect of catalyst, be not described in detail in this.
Claims (10)
1. a glass furnace denitrating catalyst, by weight, comprising:
TiO
250-60 part,
Ammonium metavanadate 0.5-2 part,
Ammonium heptamolybdate or ammonium paratungstate 2-5 part,
Ammoniacal liquor 1-2 part,
Deionized water 25-30 part,
Source of iron 1-5 part,
Cerium source 0.5-3 part,
Other additives 5-10 part, other additives are selected from potter's clay, glass, CMC, or potter's clay, glass, paper fibre, or potter's clay, glass, paper fibre, CMC.
2. glass furnace denitrating catalyst as claimed in claim 1, it is characterized in that, the mass concentration of described ammoniacal liquor is 0.091-0.227g/ml.
3. glass furnace denitrating catalyst as claimed in claim 1, it is characterized in that, described source of iron comprises the iron oxide of not sulfur-bearing, not the ferrous oxide of sulfur-bearing or ferric nitrate; Described cerium source comprises cerous nitrate or cerium oxide.
4. glass furnace denitrating catalyst as claimed in claim 1, it is characterized in that, the mass concentration of described ammoniacal liquor is 0.227g/ml, and described source of iron is the iron oxide of not sulfur-bearing, and described cerium source is cerium oxide.
5. glass furnace denitrating catalyst as claimed in claim 1, it is characterized in that, described glass furnace denitrating catalyst is by TiO
260 parts, ammonium metavanadate 2 parts, ammonium heptamolybdate or ammonium paratungstate 5 parts, ammoniacal liquor 2 parts, deionized water 30 parts, iron oxide 2 parts, cerium oxide 1 part, 4 parts, potter's clay, glass 2 parts, CMC1 part forms.
6. the preparation method of the arbitrary described glass furnace denitrating catalyst of claim 1-5, concrete steps are as follows:
1) by TiO
2, ammonium heptamolybdate or ammonium paratungstate add a part of deionized water after being dry mixed 5-10min, stir 10-20min;
2) add ammonium metavanadate, stir 10-20min;
3) add ammoniacal liquor when adding source of iron and cerium source simultaneously, stir 20-30min; Add other additives, stir 10-20min;
4) add residue deionized water, reverse agitating function mixes, and hydrofuge, obtains mixture pug.
7. preparation method as claimed in claim 6, is characterized in that, step 1) in by TiO
2, ammonium heptamolybdate or ammonium paratungstate drop in mixing roll or kneader and are dry mixed.
8. preparation method as claimed in claim 6, is characterized in that, step 1), 2) and 3) middle mixing speed 450-750 rev/min.
9. preparation method as claimed in claim 6, is characterized in that, step 3) in, the addition sequence of source of iron and cerium source and other additives is not fixed.
10. preparation method as claimed in claim 6, is characterized in that, also comprise: use extruder or coating line to make honeycomb type denitrification catalyst or plate-type denitration catalyst mixture pug, and at 520-560 degree calcining 4-8 hour.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106492783A (en) * | 2016-11-30 | 2017-03-15 | 易能环境技术有限公司 | A kind of glass furnace fume SCR denitration and preparation method thereof |
| CN108855120A (en) * | 2018-04-28 | 2018-11-23 | 中国建筑材料科学研究总院有限公司 | Monoblock type metal composite oxide low-temperature denitration catalyst and preparation method thereof |
| CN110721701A (en) * | 2019-10-16 | 2020-01-24 | 山东大学 | Cobalt-chromium modified catalyst and preparation method and application thereof |
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| CN102658161A (en) * | 2012-04-18 | 2012-09-12 | 山东大学 | Supported iron-based composite oxide catalyst and preparation method thereof |
| CN103894182A (en) * | 2014-04-01 | 2014-07-02 | 李灏呈 | Flue gas denitrification catalyst with wide activity temperature interval as well as preparation method thereof |
| CN104368334A (en) * | 2014-09-28 | 2015-02-25 | 王丽娜 | Denitration catalyst and its preparation method |
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| US20120184429A1 (en) * | 2010-03-11 | 2012-07-19 | Johnson Matthey Public Limited Company | DISORDERED MOLECULAR SIEVE SUPPORTS FOR THE SELECTIVE CATALYTIC REDUCTION OF NOx |
| CN102658161A (en) * | 2012-04-18 | 2012-09-12 | 山东大学 | Supported iron-based composite oxide catalyst and preparation method thereof |
| CN103894182A (en) * | 2014-04-01 | 2014-07-02 | 李灏呈 | Flue gas denitrification catalyst with wide activity temperature interval as well as preparation method thereof |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN106492783A (en) * | 2016-11-30 | 2017-03-15 | 易能环境技术有限公司 | A kind of glass furnace fume SCR denitration and preparation method thereof |
| CN108855120A (en) * | 2018-04-28 | 2018-11-23 | 中国建筑材料科学研究总院有限公司 | Monoblock type metal composite oxide low-temperature denitration catalyst and preparation method thereof |
| CN110721701A (en) * | 2019-10-16 | 2020-01-24 | 山东大学 | Cobalt-chromium modified catalyst and preparation method and application thereof |
| CN110721701B (en) * | 2019-10-16 | 2020-08-18 | 山东大学 | Cobalt-chromium modified catalyst and preparation method and application thereof |
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Application publication date: 20151216 |