CN101391178B - Method for removing mercury in flue gas using V2O5/carbon material catalyst - Google Patents
Method for removing mercury in flue gas using V2O5/carbon material catalyst Download PDFInfo
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- CN101391178B CN101391178B CN2008100796576A CN200810079657A CN101391178B CN 101391178 B CN101391178 B CN 101391178B CN 2008100796576 A CN2008100796576 A CN 2008100796576A CN 200810079657 A CN200810079657 A CN 200810079657A CN 101391178 B CN101391178 B CN 101391178B
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Abstract
Disclosed is a method for applying a V2O5/carbon material catalyst to remove mercury in flue gas, which comprises: feeding the catalyst into a fixed bed reactor, controlling the reaction temperature at between 120 and 180DEG C, and inputting atmospheric mercury-bearing flue gas, wherein, the concentration of mercury is 0.5 to 3070mu g/m3, and the air speed ranges from 10000 to 100000h-1; and the catalyst is the V2O5/carbon material catalyst, and has the compositions, in weight percentage: 90 to 99.5 percent of carbon material, and 0.5 to 10 percent of vanadium oxide by taking V2O5 as a unit of measurement. The invention has the advantages of rather high catalytic oxidation removal capability to mercury, reducing the running cost and solving the secondary pollution.
Description
Technical field
The present invention relates to a kind of method that removes element mercury in the flue gas, specifically relate to a kind of Application V
2O
5The method of mercury in the/carbon material catalyst catalytic oxidative desulfurization flue gas.
Background technology
Coal is the main energy sources of China, and is in recent years along with Chinese economic development, also increasing to the utilization of coal.The problem of environmental pollution that causes thus is also more outstanding, has had a strong impact on ecological environment and health and economic sustainable development.Therefore, efficiently solve the important content that the pollution that caused by coal burning problem is China's energy sustainable development.Mercury is one of harmful heavy metal pollutant of coal combustion release, and environment and people's cognition are caused very big harm.Carry out correlative study though developed country has dropped into huge fund, do not form cost-effective control technology at present as yet.
The form of mercury mainly contains the Hg of gaseous state in the coal-fired flue-gas
0And Hg
2+And the Hg of particulate form
pWherein, most of Hg
pCan be removed by electric cleaner or sack cleaner with flying dust; Hg
2+Soluble in water, can more easily be removed through wet dust removal or wet desulphurization device; Hg
0Because it has high volatile volatile and is insoluble in characteristics such as water, is difficult to removed by existing pollutant control device, thereby becomes the emphasis that coal-fired flue-gas removes research and development.
For Hg
0Emission control, at present the main method of research and development is in flue, to spray into the adsorptive gaseous mercury of active carbon powder.But active carbon is under higher flue-gas temperature, and its adsorption capacity is lower.Particularly adopt the mode that sprays into, the time that active carbon contacts with flue gas is shorter, makes that the utilization rate of active carbon is low, straying quatity is big; Not only to consume a large amount of active carbons; Raise the cost, and cause the carbon content of ash to increase, make it be difficult to satisfy the requirement of construction material.
Summary of the invention
The objective of the invention is deficiency, a kind of Application V is provided to existing mercury pollution control technology
2O
5The method of mercury efficiently removes the mercury in the flue gas in the/carbon material catalyst catalytic oxidative desulfurization flue gas, and environment is not caused secondary pollution.
For realizing this purpose, in the technical scheme of the present invention, adopt patent of invention " a kind of catalyst and method for making and purposes that removes flue gas nitrogen oxide ", the patent No. is V in 99104246.8
2O
5/ carbon material catalyst, its percentage by weight consists of: raw material of wood-charcoal material 90-99.5%, barium oxide is (with V
2O
5Be measurement unit) 0.5-10%.
Described raw material of wood-charcoal material is for comprising active carbon, activated coke or NACF
V
2O
5/ carbon material catalyst preparation method puts into absorbent charcoal material the vanadium solution that contains of 0.05-1 mol, flooded 1-20 hour, or with ion-exchange and precipitation method dipping; Then in 110 ℃ of dryings 12 hours; Under air or inert atmosphere, calcined 2-10 hour, and promptly got catalyst for 250-600 ℃.
Catalyst applications method of the present invention is that catalyst is loaded in the fixed bed reactors, and 120-180 ℃ of control reaction temperature feeds the normal pressure mercury fume, and wherein the concentration of mercury is 0.5-3070 μ g/m
3, air speed 10000-100000h
-1
The present invention compared with prior art has the following advantages:
1, adopt fixed bed reactors, flue gas can with the catalyst even contact, increased time of contact, the demercuration ability of catalyst can be made full use of.
2, supported V
2O
5To activated coke, promoted mercury catalytic oxidation above that, significantly improved its ability that removes to mercury, and SO in the flue gas
2Not only, on the contrary its demercuration there is obvious facilitation to the nontoxic usefulness that turns into of catalyst.
3, catalyst is renewable recycles, and has reduced cost, has solved the secondary pollution problem.
The specific embodiment
Embodiment 1
1 gram activated coke is with the NH of 1 milliliter of 0.1 mol
4VO
3-H
2C
2O
4Solution impregnation 10 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 500 ℃ of calcinings 2 hours promptly get 1wt%V
2O
5/ activated coke catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 120 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 10000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 6.3%O
2, 6%H
2O, 1500ppm SO
2, N
2Be balance gas, Hg
0Concentration is 420 μ g/m
3Equally, carried out the active carbon demercuration experiment under the same terms as a comparison.Experimental result is: catalyst reaches 206 μ g/g-catalyst in the suction mercury amount of 24h, and the suction mercury amount of active carbon is 19 μ g/g-active carbons.
Embodiment 2
1 gram activated coke is with the NH of 1 milliliter of 0.05 mol
4VO
3-H
2C
2O
4Solution impregnation 2 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 450 ℃ of calcinings 5 hours promptly get 0.5wt%V
2O
5/ activated coke catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 120 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 15000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 6.3%O
2, 6%H
2O, 1000ppm SO
2, N
2Be balance gas, Hg
0Concentration is 420 μ g/m
3Experimental result is: catalyst reaches 140 μ g/g-catalyst in the suction mercury amount of 24h.
Embodiment 3
1 gram NACF
NH with 1 milliliter of 0.5 mol
4VO
3-H
2C
2O
4Solution impregnation 5 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 350 ℃ of calcinings 10 hours promptly get 5wt%V
2O
5/ NACF catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 120 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 10000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 6.3%O
2, 6%H
2O, 1500ppm SO
2, N
2Be balance gas, Hg
0Concentration is 420 μ g/m
3Experimental result is: catalyst reaches 234 μ g/g-catalyst in the suction mercury amount of 24h.
Embodiment 4
1 gram activated coke is with the NH of 1 milliliter of 1 mol
4VO
3-H
2C
2O
4Solution impregnation 8 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 600 ℃ of calcinings 7 hours promptly get 10wt%V
2O
5/ activated coke catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 120 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 10000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 5%O
2, 4%H
2O, 1500ppm SO
2, N
2Be balance gas, Hg
0Concentration is 870 μ g/m
3Experimental result is: catalyst reaches 468 μ g/g-catalyst in the suction mercury amount of 24h.
Embodiment 5
1 gram active carbon is with the NH of 1 milliliter of 0.1 mol
4VO
3-H
2C
2O
4Solution impregnation 12 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 300 ℃ of calcinings 2 hours promptly get 1wt%V
2O
5/ activated-carbon catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 150 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 10000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 6% O
2, 3% H
2O, 1200ppm SO
2, N
2Be balance gas, Hg
0Concentration is 420 μ g/m
3Experimental result is: catalyst reaches 252 μ g/g-catalyst in the suction mercury amount of 24h.
Embodiment 6
1 gram activated coke is with the NH of 1 milliliter of 0.1 mol
4VO
3-H
2C
2O
4Solution impregnation 15 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 400 ℃ of calcinings 5 hours promptly get 1wt%V
2O
5/ activated coke catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 180 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 10000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 6.3%O
2, 6%H
2O, 1500ppmSO
2, N
2Be balance gas, Hg
0Concentration is 420 μ g/m
3Experimental result is: catalyst reaches 231 μ g/g-catalyst in the suction mercury amount of 24h.
Embodiment 7
1 gram activated coke is with the NH of 1 milliliter of 0.1 mol
4VO
3-H
2C
2O
4Solution impregnation 15 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 500 ℃ of calcinings 5 hours promptly get 1wt%V
2O
5/ activated coke catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 120 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 10000h
-1, constant temperature absorption 200h, it is saturated to make catalyst inhale mercury.Simulated flue gas consists of: 6.3%O
2, 6%H
2O, 150OppmSO
2, N
2Be balance gas, Hg
0Concentration is 3070 μ g/m
3Experimental result is: the saturated suction mercury amount of catalyst reaches 3042 μ g/g-catalyst.
Embodiment 8
1 gram activated coke is with the NH of 1 milliliter of 0.1 mol
4VO
3-H
2C
2O
4Solution impregnation 10 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 500 ℃ of calcinings 5 hours promptly get 1wt%V
2O
5/ activated coke catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 120 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 30000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 6.3%O
2, 6%H
2O, 1500ppm SO
2, N
2Be balance gas, Hg
0Concentration is 10 μ g/m
3Experimental result is: catalyst reaches 5.8 μ g/g-catalyst in the suction mercury amount of 24h.
Embodiment 9
1 gram activated coke is with the NH of 1 milliliter of 0.2 mol
4VO
3-H
2C
2O
4Solution impregnation 10 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 500 ℃ of calcinings 5 hours promptly get 2wt%V
2O
5/ activated coke catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 120 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 100000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 6.3%O
2, 6%H
2O, 1500ppmSO
2, N
2Be balance gas, Hg
0Concentration is 1020 μ g/m
3Experimental result is: catalyst reaches 135 μ g/g-catalyst in the suction mercury amount of 24h.
Embodiment 10
1 gram activated coke is with the NH of 1 milliliter of 0.1 mol
4VO
3-H
2C
2O
4Solution impregnation 10 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 500 ℃ of calcinings 5 hours promptly get 1wt%V
2O
5/ activated coke catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 120 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 10000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 6.3%O
2, N
2Be balance gas, Hg
0Concentration is 420 μ g/m
3Experimental result is: catalyst reaches 125 μ g/g-catalyst in the suction mercury amount of 24h.
Embodiment 11
1 gram activated coke is with the NH of 1 milliliter of 0.1 mol
4VO
3-H
2C
2O
4Solution impregnation 10 hours, then in 110 ℃ of dryings 12 hours, under argon gas atmosphere, 500 ℃ of calcinings 5 hours promptly get 1wt%V
2O
5/ activated coke catalyst.
This catalyst is filled in the fixed bed quartz tube reactor, and two ends are fixed with silica wool.Catalyst is warming up to 120 ℃ in reactor after, begins feeding and contain Hg
0Simulated flue gas, air speed 10000h
-1, constant temperature absorption 24h.Simulated flue gas consists of: 6.3%O
2, 1500ppmSO
2, N
2Be balance gas, Hg
0Concentration is 420 μ g/m
3Experimental result is: catalyst reaches 185 μ g/g-catalyst in the suction mercury amount of 24h.
Claims (1)
1. Application V
2O
5/ carbon material catalyst removes the method for mercury in the flue gas, it is characterized in that comprising the steps:
Catalyst is loaded in the fixed bed reactors, and 120-180 ℃ of control reaction temperature feeds the normal pressure mercury fume, and wherein the concentration of mercury is 0.5-3070 μ g/m
3, air speed 10000-100000h
-1
Described catalyst is V
2O
5/ carbon material catalyst, its percentage by weight are formed: raw material of wood-charcoal material 90-99.5%, and with V
2O
5Be measurement unit barium oxide 0.5-10%;
Described raw material of wood-charcoal material is active carbon, activated coke or NACF.
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|---|---|---|---|
| CN2008100796576A CN101391178B (en) | 2008-10-24 | 2008-10-24 | Method for removing mercury in flue gas using V2O5/carbon material catalyst |
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|---|---|---|---|
| CN2008100796576A CN101391178B (en) | 2008-10-24 | 2008-10-24 | Method for removing mercury in flue gas using V2O5/carbon material catalyst |
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| CN101391178B true CN101391178B (en) | 2012-07-25 |
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| CN103143320B (en) * | 2013-03-12 | 2014-09-17 | 山东科技大学 | Active carbon/zeolite shaped composite material for removing elemental mercury in coal-burned flue gas and preparation method thereof |
| CN103521164B (en) * | 2013-10-18 | 2015-07-15 | 东南大学 | Flue gas demercuration, desulfurization and denitration adsorbent and preparation method thereof |
| CN104549273A (en) * | 2014-12-31 | 2015-04-29 | 北京北华中清环境工程技术有限公司 | Metal oxide loading active carbon catalyst and preparation method thereof |
| CN106237982A (en) * | 2016-10-25 | 2016-12-21 | 安庆师范大学 | CuO/ attapulgite catalyst-sorbent and for removing the method for Elemental Mercury in flue gas |
| CN108993504B (en) * | 2018-07-25 | 2021-12-14 | 北京市劳动保护科学研究所 | Modified activated coke for demercuration of sulfur-containing flue gas and preparation method thereof |
| CN110252367B (en) * | 2019-05-06 | 2022-01-11 | 江苏大学 | Solvothermal method for preparing few-layer carbon nitride supported vanadium dioxide catalyst and desulfurization application thereof |
| CN113198444A (en) * | 2021-05-12 | 2021-08-03 | 昆明理工大学 | Low-temperature CO reduction denitration V/AC catalyst and preparation method and application thereof |
| CN113663641A (en) * | 2021-08-24 | 2021-11-19 | 航天环境工程有限公司 | Preparation method and application of novel mercury removal adsorbent |
| CN114789051B (en) * | 2022-04-02 | 2023-12-12 | 中国科学院山西煤炭化学研究所 | Desulfurization, denitrification and vanadium carbon catalyst regeneration method for reducing dioxin release |
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