CN1792455A - Cellular activated-carbon catalyst used for denitrification of flue-gas, prepn. method and application thereof - Google Patents
Cellular activated-carbon catalyst used for denitrification of flue-gas, prepn. method and application thereof Download PDFInfo
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- CN1792455A CN1792455A CN200510048251.8A CN200510048251A CN1792455A CN 1792455 A CN1792455 A CN 1792455A CN 200510048251 A CN200510048251 A CN 200510048251A CN 1792455 A CN1792455 A CN 1792455A
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Abstract
一种用于烟气脱氮的蜂窝状活性炭催化剂是由蜂窝状活性炭与活性组分组成，其重量百分比组成为：蜂窝状活性炭92－99.5％，活性组分0.5－8％，活性成分是铁、锰、钒的一种或几种金属氧化物。采用等体积法浸渍法制备。对烟气进行脱硝的方法是催化剂填装在反应器中，反应温度控制在120－250℃，操作空速为500－3000h－1的条件下进行。本发明具有净化效率高、无二次污染、床层阻力低等特点。可用于工业尾气的治理，尤其适用于大风量锅炉烟气、硝酸尾气的治理的优点。A honeycomb activated carbon catalyst for flue gas denitrification is composed of honeycomb activated carbon and active components, and its weight percentage is: honeycomb activated carbon 92-99.5%, active components 0.5-8%, active components are iron One or several metal oxides of manganese and vanadium. Prepared by isometric impregnation method. The method for denitrifying the flue gas is that the catalyst is filled in the reactor, the reaction temperature is controlled at 120-250° C., and the operating space velocity is 500-3000h -1 . The invention has the characteristics of high purification efficiency, no secondary pollution, low bed resistance and the like. It can be used for the treatment of industrial tail gas, especially suitable for the treatment of large air volume boiler flue gas and nitric acid tail gas.
Description
Technical field
The invention belongs to a kind of catalyst and method for making and application, relate in particular to a kind of cellular activated-carbon catalyst and method for making and application that is used for flue-gas denitrification.
Technical background
China is coal-fired big country, and coal fire discharged sulfur dioxide and nitrogen oxide are increasing year by year, become the primary pollution source of atmospheric environment.Flue gas desulfurization technique research early, technology is comparative maturity also, and the gas denitrifying technology exploitation is later, has taked at present such as low nitrogen oxide burner, staged air distribution, OFA (Over Fire Air), technical measures reduction NO such as combustion again
XDischarging, obtained certain effect, but along with the improving constantly of environmental requirement, discharge standard from now on is more and more stricter, takes abovementioned technology often to be difficult to reach discharge index.With ammonia is SCR (SCR) technology of reducing agent, because its higher NO
XRemoval efficiency is obtaining application more and more widely, but high temperature SCR technology has limited it and applied because its expensive catalysts and life problems have caused investment excessive.And denitration reaction can be realized at low temperature (100-250 ℃) through chemically treated active carbon in the surface, is suitable for the exhaust gas temperature of most of boiler, and denitration efficiency can be adjusted air speed design according to flue-gas temperature.Active carbon low-temperature SCR technology has low, the advantage such as consume water, non-secondary pollution not of operating cost, in addition, honeycombed catalyst have bed resistance little, can overcome advantages such as dust obstruction, so cellular activated-carbon catalyst has wide practical use aspect low-temperature denitration of flue gas.
Summary of the invention
The purpose of this invention is to provide a kind of cellular activated-carbon catalyst and methods for making and using same that can efficiently remove nitrogen oxide at low temperatures.
Catalyst of the present invention is made up of Alveolate activated carbon capable and active component, and its percentage by weight consists of: Alveolate activated carbon capable 92-99.5%, active component 0.5-8%, active component are one or more metal oxides of iron, manganese, vanadium.
Aforesaid Alveolate activated carbon capable is by being mixed into the plasticity material by coal dust and adhesive, and extrusion molding then, drying, charing, steam activation obtain, and concrete making step sees that application number is 200410092429.4 patent of invention.
Preparation of catalysts method of the present invention is that the salt with one or more metal active compositions of iron, manganese, vanadium is mixed with solution, adopts equi-volume process dipping Alveolate activated carbon capable, and drying, calcining, oxidation obtain then.
Aforesaid molysite or manganese salt are nitrate, and vanadic salts is an ammonium metavanadate.
Catalyst application process of the present invention makes catalyst filling in reactor, and reaction temperature is controlled at 120-250 ℃, feeds flue gas, and the operation air speed is 500-3000h
-1Condition under carry out denitration, NO
XConversion ratio reaches 50-95%.
Advantage of the present invention is:
Have characteristics such as purification efficiency height, non-secondary pollution, bed resistance be low.Can be used for the improvement of industrial tail gas, be particularly useful for the improvement of big air quantity boiler smoke, nitric acid tail gas.
The specific embodiment
Embodiment 1:
1, preparation Alveolate activated carbon capable
(1) coal dust configuration: brown coal and coking coal are crushed to respectively≤2mm, then by quality than brown coal: after coking coal=mixing in 1: 0.3, be ground to below the 74 μ m coal dust that obtains mixing again.
(2) emulsification coal tar: the first step, bitumen content are that 57% high temperature coal-tar is preheated to 120 ℃; Second step, the preparation emulsifier aqueous solution.Add 4% surfactant (is benchmark with coal tar) and 0.5% stabilizing agent (is benchmark with coal tar) in the water, and be preheated to 80 ℃ and form emulsifier aqueous solutions; In the 3rd step, press high temperature coal-tar: emulsifier aqueous solution (mass ratio)=1: 0.5 slowly adds coal tar under stirring condition and makes emulsification coal tar in the emulsifier aqueous solution.The surfactant of emulsification high temperature coal-tar is a sodium lignin sulfonate, and stabilizing agent is a calcium chloride.
(3) processing of plasticity coal slime: coal dust in proportion: emulsification coal tar: water: polyvinyl alcohol: tung oil=38: 36: 20: add in kneaders at 4: 2 and to stir, make plastic coal slime.
(4) pugging: the plasticity coal slime is handled through vacuum deairing machine or extrusion shaping machine, and coal slime is mixed, and removes the large particulate matter that above-mentioned operation may be brought into 60 purpose silk screen filter then in make-up machine.
(5) extrusion molding: the coal slime adding after pugging is handled is equipped with in the extrusion shaping machine of honeycomb steel mold, is to carry out moulding, the honeycomb ceramics that obtains wetting under the 7Mpa in briquetting pressure.
(6) drying: wet honeycomb ceramics is dried to moisture and is lower than 2%.
(7) charing and activation: as protection gas, be heated to 600 ℃ with nitrogen or argon gas by 3 ℃/min of programming rate, and charing 2 hours under this temperature; Being warmed up to 800 ℃ by 5 ℃/min of programming rate then, is activated media activation 10 hours with steam, obtains Alveolate activated carbon capable.
2, preparation cellular activated-carbon catalyst and application
The ammonium metavanadate solution of configuration 0.01g/ml; adopt equi-volume process dipping Alveolate activated carbon capable carrier; place 2h; in 120 ℃ of dry 3h; under nitrogen protection, calcine 4h in 500 ℃; then in air in 250 ℃ of oxidation 8h, obtain the cellular activated-carbon catalyst that pentoxide content is 0.5% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 120 ℃, and air speed is 500h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen are balance gas, with 500ppm NH
3Be reducing agent, the NO conversion ratio is 80% under this operating condition.
Embodiment 2:
The ammonium metavanadate solution of configuration 0.02g/ml; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection, calcine 4h in 500 ℃; then in air in 250 ℃ of oxidation 8h, obtain the cellular activated-carbon catalyst that pentoxide content is 1.0% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 120 ℃, and air speed is 1200h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen is balance gas, with 500ppmNH
3Be reducing agent, the NO conversion ratio is 60% under this operating condition.
Embodiment 3:
The ammonium metavanadate solution of configuration 0.04g/ml; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection, calcine 4h in 500 ℃; then in air in 250 ℃ of oxidation 8h, obtain the cellular activated-carbon catalyst that pentoxide content is 2.0% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 200 ℃, and air speed is 1200h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen is balance gas, with 500ppmNH
3Be reducing agent, the NO conversion ratio is 78% under this operating condition.
Embodiment 4:
The ammonium metavanadate solution of configuration 0.05g/ml; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection, calcine 4h in 500 ℃; then in air in 250 ℃ of oxidation 8h, obtain the cellular activated-carbon catalyst that pentoxide content is 2.5% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 250 ℃, and air speed is 2000h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen is balance gas, with 500ppmNH
3Be reducing agent, the NO conversion ratio is 65% under this operating condition.
Embodiment 5:
The manganese nitrate solution of configuration 0.043g/ml; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection, calcine 3h in 200 ℃; then in air in 250 ℃ of oxidation 5h, obtain the cellular activated-carbon catalyst that manganese dioxide content is 4.5% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 120 ℃, and air speed is 1200h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen are balance gas, with 500ppm NH
3Be reducing agent, the NO conversion ratio is 65% under this operating condition.
Embodiment 6:
The manganese nitrate solution of configuration 0.018g/ml; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection, calcine 3h in 200 ℃; then in air in 250 ℃ of oxidation 10h, obtain the cellular activated-carbon catalyst that manganese dioxide content is 2% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 150 ℃, and air speed is 1800h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen are balance gas, with 500ppm NH
3Be reducing agent, the NO conversion ratio is 85% under this operating condition.
Embodiment 7:
The iron nitrate solution of configuration 0.013g/ml; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection, calcine 3h in 200 ℃; then in air in 250 ℃ of oxidation 8h, obtain the cellular activated-carbon catalyst that ferric oxide content is 4% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 120 ℃, and air speed is 1200h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen is balance gas, with 500ppmNH
3Be reducing agent, the NO conversion ratio is 57% under this operating condition.
Embodiment 8:
The iron nitrate solution of configuration 0.026g/ml; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection, calcine 4h in 200 ℃; then in air in 250 ℃ of oxidation 8h, obtain the cellular activated-carbon catalyst that ferric oxide content is 8% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 200 ℃, and air speed is 1800h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen are balance gas, with 500ppm NH
3Be reducing agent, the NO conversion ratio is 70% under this operating condition.
Embodiment 9:
The iron nitrate solution of configuration 0.0066g/ml; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection, calcine 4h in 500 ℃; then in air in 250 ℃ of oxidation 8h, obtain the cellular activated-carbon catalyst that ferric oxide content is 2% (percentage by weight).Get length and place reactor (Ф 20mm) for the 50mm catalyst, the control reaction temperature is at 250 ℃, and air speed is 2000h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen is balance gas, with 500ppmNH
3Be reducing agent, the NO conversion ratio is 90% under this operating condition.
Embodiment 10:
Manganese nitrate 0.043g, ferric nitrate 0.66g join in the 100ml water; be configured to solution; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection in 500 ℃ the calcining 4h, then in air in 250 ℃ of oxidation 8h, obtain MnO
2, Fe
2O
3Content is respectively the cellular activated-carbon catalyst of 1%, 2% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 150 ℃, and air speed is 1500h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen are balance gas, with 500ppm NH
3Be reducing agent, the NO conversion ratio is 84% under this operating condition.
Embodiment 11:
Ferric nitrate 0.66g, ammonium metavanadate 2g join in the 100ml water; be configured to solution; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection in 500 ℃ the calcining 4h, then in air in 250 ℃ of oxidation 8h, obtain Fe
2O
3, V
2O
5Content is respectively the cellular activated-carbon catalyst of 2%, 1% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 200 ℃, and air speed is 2000h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4%H
2O, nitrogen are balance gas, with 500ppm NH
3Be reducing agent, the NO conversion ratio is 90% under this operating condition.
Embodiment 11:
Manganese nitrate 0.043g, ferric nitrate 0.66g, ammonium metavanadate 2g join in the 100ml water; be configured to solution; adopt equi-volume process dipping Alveolate activated carbon capable carrier (preparation of absorbent charcoal carrier is with embodiment 1); place 2h; in 120 ℃ of dry 3h; under nitrogen protection in 500 ℃ the calcining 4h, then in air in 250 ℃ of oxidation 8h, obtain MnO
2, Fe
2O
3, V
2O
5Content is respectively the cellular activated-carbon catalyst of 1%, 2%, 1% (percentage by weight).Get length and place reactor (Φ 20mm) for the 50mm catalyst, the control reaction temperature is at 250 ℃, and air speed is 3000h
-1, simulated flue gas consists of 500ppm NO, 4% O
2, 3.4% H
2O, nitrogen are balance gas, with 500ppm NH
3Be reducing agent, the NO conversion ratio is 95% under this operating condition.
Claims (5)
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