CN103566928A - Manganese peroxide loaded active carbon fiber for removing NOx at room temperature and preparation method thereof - Google Patents
Manganese peroxide loaded active carbon fiber for removing NOx at room temperature and preparation method thereof Download PDFInfo
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- CN103566928A CN103566928A CN201310542796.9A CN201310542796A CN103566928A CN 103566928 A CN103566928 A CN 103566928A CN 201310542796 A CN201310542796 A CN 201310542796A CN 103566928 A CN103566928 A CN 103566928A
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Abstract
The invention discloses a manganese peroxide loaded active carbon fiber and a preparation method thereof, and aims at providing an active carbon fiber which achieves the synergetic effect of manganese peroxide and an active carbon fiber by taking the active carbon fiber as a carrier and the loaded manganese peroxide as a catalyst, has the capacity of carrying out catalytic oxidation on low-concentration NO at room temperature and then further removes NOx. The preparation method comprises the following steps of: soaking the active carbon fiber into a manganous water solution with certain concentration; then dropping a potassium permanganate water solution with certain concentration, wherein potassium permanganate and manganous generate oxidation-reduction reaction, and generated manganese peroxide is deposited on the surface of the active carbon fiber and in a micropore, so that the manganese peroxide loaded active carbon fiber is prepared. The manganese peroxide loaded active carbon fiber prepared through the method disclosed by the invention has higher removal capacity on the NOx at room temperature.
Description
Technical field
The invention belongs to the preparation method of a kind of new material and this material, relate to NACF for the load manganese dioxide of NO_x removal under room temperature and preparation method thereof.
Background technology
Take nitric oxide and nitrogen dioxide as main nitrogen oxide (NOx) is one of air-polluting main component, is to form one of serious problem of environmental pollution major reason such as acid rain, photochemical fog and gray haze, the serious threat mankind and vegeto-animal health.Therefore, the improvement of nitrogen oxide is very urgent.At present, the method for NO_x removal can be divided into on-catalytic method and the large class of catalysis method two.The former comprises absorption process, absorption method etc., has that equipment is huge, cost is high, secondary pollution problems.The latter's catalysis method mainly contains catalytic reduction and catalytic oxidation, for the catalyst in catalysis method, has the problem of poor activity, although some noble metal activity are higher, noble metal is expensive, resource scarcity, and can only be at the temperature far above room temperature effectively.
At present, the catalyst material that can be used in catalytic oxidation NO under room temperature is mainly material with carbon element, comprises active carbon, NACF, porous charcoal nanofiber etc.Chinese patent ZL201110396801.0 has reported the removal effect that porous charcoal nanofiber prepared by method of electrostatic spinning has at room temperature had the NO of low concentration.But because carbon nanofibers preparation cost is high, be difficult to large-scale application.And active carbon is owing to being graininess, for the improvement of NOx in air, there is mounting design difficulty, the problem such as efficiency is low.Comprehensively by comparison, in these several Carbon Materials, what be hopeful large-scale application most is NACF, and this has benefited from it and has larger specific area, fiber condition and moderate preparation cost.
We are used for removing of room temperature low concentration of NO by asphalt based active carbon fiber, and discovery can be by NO catalytic oxidation (Journal of Chemical Industry and Engineering, 2011,62 (2): 369-373), but Catalytic Oxygen rate is on the low side.For further improving its catalytic oxidation activity, strengthen the ability that removes to NOx, need be on NACF supported catalyst.
Summary of the invention
In order further to improve the catalytic oxidation efficiency to low concentration of NO under NACF room temperature, the present invention adopts coprecipitation load manganese dioxide to NACF, utilize that manganese dioxide source is abundant, cheap, safety non-toxic, there is the higher advantages such as catalytic activity, the NACF of preparation load manganese dioxide, low concentration of NO in air is adsorbed and catalytic oxidation, and and then remove.
To achieve these goals, the technical solution used in the present invention is:
The load of usining has the NACF of manganese dioxide as the catalyst of low concentration of NO, utilizes the concerted catalysis effect of NACF and manganese dioxide, and it is NO that the NO of low concentration under room temperature is carried out to catalytic oxidation
2, more further remove.
The present invention also provides described and has utilized chemical coprecipitation technique for removing the preparation method of NACF of the load manganese dioxide of air NOx, by manganese dioxide load to NACF.
Under room temperature, remove a NACF for the load manganese dioxide of air low concentration of NO x, take NACF as carrier, the manganese dioxide of load quality mark 0.001-5%.
Described NACF is polyacrylonitrile-radical, viscose base, asphaltic base or phenolic aldehyde base, and specific area is 500-2000m
2/ g.
The mass fraction of described manganese dioxide is 0.6%, 1.8%, 2.6%, 3.6% or 4.3%.
A preparation method for the NACF of load manganese dioxide, take NACF as carrier, utilizes coprecipitation, comprises the following steps:
Step 4, is placed in nitrogen atmosphere stove by the NACF obtaining in step 3, from room temperature, rises to 200-300 ℃, cools to room temperature with the furnace after being then incubated a period of time.
Coprecipitation manganous salt used in described step 1 is the water-soluble manganese salts such as manganese nitrate, manganese sulfate or manganese acetate.
In described step 2, dip time is at least 10 minutes
In described step 4, temperature retention time is at least 1 hour.
Compared with prior art, the NACF of the load manganese dioxide of preparing by the present invention at room temperature has the stronger ability that removes to NOx, can make NO Catalytic Oxygen rate more than 27%, reaches as high as 31%.
Accompanying drawing explanation
NACF ESEM (SEM) figure of Fig. 1 load manganese dioxide.
Relation on Fig. 2 NACF between manganese dioxide load amount and NO Catalytic Oxygen rate.
The specific embodiment
Below in conjunction with the specific embodiment, the present invention is further elaborated.In the situation that not departing from the above-mentioned thought of the present invention, various replacements or the change according to ordinary skill knowledge and customary means, made, all within the scope of the present invention.
Embodiment mono-
Preparation method for the NACF of the load manganese dioxide of room temperature NO_x removal, utilizes coprecipitation load manganese dioxide to NACF, comprises the following steps:
Step 4, is placed in nitrogen atmosphere stove by the NACF obtaining in step 3, from room temperature, rises to 200 ℃, cools to room temperature with the furnace after being then incubated 4h.
Obtain the NACF of load 0.6% manganese dioxide.
Embodiment bis-
Preparation method for the NACF of the load manganese dioxide of room temperature NO_x removal, utilizes coprecipitation load manganese dioxide to NACF, comprises the following steps:
Step 4, is placed in nitrogen atmosphere stove by the NACF obtaining in step 3, from room temperature, rises to 300 ℃, cools to room temperature with the furnace after being then incubated 2h.
Obtain the NACF of load 1.8% manganese dioxide.
Embodiment tri-
Preparation method for the NACF of the load manganese dioxide of room temperature NO_x removal, utilizes coprecipitation load manganese dioxide to NACF, comprises the following steps:
Step 4, is placed in nitrogen atmosphere stove by the NACF obtaining in step 3, from room temperature, rises to 300 ℃, cools to room temperature with the furnace after being then incubated 3h.
Obtain the NACF of load 2.6% manganese dioxide.
Embodiment tetra-
Preparation method for the NACF of the load manganese dioxide of room temperature NO_x removal, utilizes coprecipitation load manganese dioxide to NACF, comprises the following steps:
Step 4, is placed in nitrogen atmosphere stove by the NACF obtaining in step 3, from room temperature, rises to 300 ℃, cools to room temperature with the furnace after being then incubated 2h.
Obtain the NACF of load 3.6% manganese dioxide.
Embodiment five
Preparation method for the NACF of the load manganese dioxide of room temperature NO_x removal, utilizes coprecipitation load manganese dioxide to NACF, comprises the following steps:
Step 4, is placed in nitrogen atmosphere stove by the NACF obtaining in step 3, from room temperature, rises to 300 ℃, cools to room temperature with the furnace after being then incubated 2h.
Obtain the NACF of load 4.3% manganese dioxide, its form as shown in Figure 1.
Utilize said method to obtain the NACF of load manganese dioxide, at room temperature low concentration of NO x is had to the stronger ability that removes.
The NACF catalytic oxidation NO method of testing of load manganese dioxide is as follows: composite active carbon fibre is dried to 12 hours at 120 ℃, to remove moisture wherein and the material of other absorption, the fiber that takes a certain amount of (0.05~0.20g) is inserted in fixed bed.Fixed bed diameter is 11mm, and packed height is 15~50mm.Low concentration of NO gas is by NO Standard Gases, O
2, N
2three kinds of gases are formulated, and its flow is controlled by mass flowmenter and regulated, and gaseous mixture total flow is 100~200SCCM.Through flowmeter Hou tri-road gases, enter mixed gas tank, after mixed gas tank mixes, enter fixed bed and carry out NO catalytic oxidation, the temperature of fixed bed is controlled by water-bath, and reacted gas enters nitrogen-oxide analyzer, (Thermo42i type) and carries out concentration determination.
By specific area, be 1500m
2the manganese dioxide of the different amounts of load on the asphalt based active carbon fiber of/g, (test condition is relation between test NO Catalytic Oxygen rate and carrying capacity: NO concentration is 50ppm, reaction temperature is 30 ℃, specimen consumption is 0.100g, packed height 6mm, gas flow rate is 200mL/min), acquired results is as shown in Figure 2.Can find out, when load 3-4.5% manganese dioxide, NO Catalytic Oxygen rate, more than 27%, reaches as high as 31%.
Claims (7)
1. for removing a NACF for the load manganese dioxide of air low concentration of NO x under room temperature, it is characterized in that, take NACF as carrier, the manganese dioxide of load quality mark 0.001-5%.
2. the NACF of load manganese dioxide described in claim 1, is characterized in that, described NACF is polyacrylonitrile-radical, viscose base, asphaltic base or phenolic aldehyde base, and specific area is 500-2000m
2/ g.
3. the NACF of load manganese dioxide described in claim 1, is characterized in that, the mass fraction of described manganese dioxide is 0.6%, 1.8%, 2.6%, 3.6% or 4.3%.
4. a preparation method for the NACF of load manganese dioxide described in claim 1, is characterized in that, take NACF as carrier, utilizes coprecipitation, comprises the following steps:
Step 1, the manganous salt aqueous solution that the potassium permanganate solution that compound concentration is 0.005-0.05mol/L and concentration are 0.005-0.05mol/L;
Step 2, is immersed in NACF in the manganous salt aqueous solution, under agitation drips the liquor potassic permanganate of same concentrations same amount after dipping certain hour under state, continues to stir to make the abundant load of product after dripping;
Step 3, is filtered dry the NACF in step 2, is placed at 90-120 ℃ and makes it dry;
Step 4, is placed in nitrogen atmosphere stove by the NACF obtaining in step 3, from room temperature, rises to 200-300 ℃, cools to room temperature with the furnace after being then incubated a period of time.
5. preparation method according to claim 4, is characterized in that, the coprecipitation manganous salt used in described step 1 is the water-soluble manganese salts such as manganese nitrate, manganese sulfate or manganese acetate.
6. preparation method according to claim 4, is characterized in that, in described step 2, dip time is at least 10 minutes.
7. preparation method according to claim 4, is characterized in that, in described step 4, temperature retention time is at least 1 hour.
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