CN107583639B - A kind of processing method for the organic exhaust gas containing chlorine - Google Patents
A kind of processing method for the organic exhaust gas containing chlorine Download PDFInfo
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Abstract
The present invention provides a kind of processing method for the organic exhaust gas containing chlorine, by the way that first reactor, second reactor and third reactor is continuously arranged, single-reactor is avoided not to be suitable for multi-component CVOCs catalysis burning bring emission technical problem not up to standard, improve the overall removal efficiency of organic exhaust gas, and catalyst activity stablizes the service life up to 300 hours or more, organochlorine exhaust gas removal efficiency is up to 99% or more.
Description
Technical field
The present invention relates to chlorine contained exhaust gas processing, in particular to a kind of processing method for the organic exhaust gas containing chlorine.
Background technique
Volatile organic compounds (VOCs) is the general designation of a kind of compound, although WHO, EU, USAEPA, ISO etc. at present
International organization, mechanism or the national definition in relation to VOCs are had different versions, but VOCs is often referred to the boiling point in 101KPa and is lower than
The organic compound of 373.15K, boiling point is lower, readily volatilized to pollute into atmosphere, be it is generally existing in air and at
Divide more complicated a kind of organic pollutant.
Volatile organic matter containing chlorine (CVOC) is a kind of important branch of VOCs, mainly includes chloromethanes (CM), dichloromethane
Alkane (DCM), vinyl chloride (VC), chlorobenzene (CB), 1,2- dichloroethanes (DCE) and trichloro ethylene (TCE) etc., these substances have
Stronger toxicity occurs photochemical reaction with nitrogen oxides under certain condition in an atmosphere, can cause surface ozone concentration
Increase, secondary organic aerosol can also be formed with some radical reactions in atmosphere by forming photochemical fog.Some chemical combination
Object then consumes stratospheric ozone, causes the Ozone hole heart, and some then can generate excessive ozone in troposphere.In addition, recently
Some bright VOCs of result of study page table can result in certain harm to human health.Therefore strong to human body based on these substances
The great influence of health and ecological environment, more and more researchers and mechanism then begin to focus on its administering method.
In view of the serious harm of the volatile organic compounds containing chlorine, making its administering method also becomes the heat of current international environment
Point problem.Nowadays it is other to be broadly divided into two major classes for CVOCs processing method: one is non-destructive techniques, also known as absorption method, can
By changing physical condition, such as temperature, pressure condition, it is enriched with CVOCs, is then separated again, this method includes absorption
Method, UF membrane, absorption process and condensation method etc..Another kind is destructive technology, by the method for chemistry or biology, makes CVOCs
It is converted into CO2、H2O and HCl etc. is nontoxic or toxic small molecule inorganic matter, and this method includes direct burning, photochemical catalytic oxidation, urges
Change burning, biodegrade etc..The applicable elements of these types of method are different, for example, absorption method has the exhaust gas of low concentration
There is good eradicating efficacy, but may cause and pollution is transferred to solid phase from gas phase, causes secondary pollution problem；Condensation method is main
High concentration, the exhaust gas of small air quantity are handled, but there is investment greatly for the exhaust gas of low concentration, Wind Volume, operating cost is high, and income is low
The disadvantages of；Directly burning processing high-concentration waste gas, but since reaction old woman spends height, substantially higher than 800 DEG C.And in combustion product
It will appear dioxin, the harmful by-products such as NOx；But catalysis burning not only has that low energy consumption under conditions of low concentration gas,
The features such as without secondary pollution and high-efficient, and be also the most effective processing method of currently commercially processing industrial waste gas it
One.
The catalyst of three types: noble metal catalyst, solid acid catalysis is concentrated mainly on for CVOCs catalysis burning
Agent, catalyst of transition metal oxide.There are prices that relatively expensive, the active height of chloro (is also easy to produce toxicity more for noble metal catalyst
Big more chloro by-products), oxychlorination easily generated closes object and is poisoned, is poisoned etc. and asks because of the loss of noble metal in high-temperature region
Topic, so that the application of noble metal catalyst is restricted.Transition-metal catalyst currently used for chlorination aromatic hydrocarbon catalysis burning
Mainly V2O5-TiO2Base catalyst etc..But V2O5-TiO2TiO in base catalyst2With toxicity, it be easy to cause secondary dirt
Dye, limits its application.Though other kinds of catalyst such as solid acid catalyst has some applications, eventually because activity is low or secondary
Product is mostly without widely being promoted.
In patent document main catalyst activity component transition metal oxide to be used be UO2, MnO2, Co3O4,
La2O3, LaO2 etc. and precious metals pt, Pd etc., carrier SiO2, Al2O3, TiO2, ZrO2.Representative patent has
JP2002219364、JP2001286729、JP2001278630、JP2001009284、JP2001286734、
JP2001327869、JP10085559A2、US4031149A、US4059677A、US4065543A、US4561969A、
US58116628A, US4169862A, US7052663A etc..
But CVOCs tail gas is frequently not a kind of single halogenated hydrocarbons, is often accompanied with other kinds of organic matter.And due to
The influence of competitive Adsorption and reaction temperature, then study one pack system CVOCs screen with high activity and selectivity technique it is different
Surely it is suitable for multi-component CVOCs.
Summary of the invention
In order to solve the technical problem, the present invention provides a kind of processing method for the organic exhaust gas containing chlorine, will contain chlorine organic waste
Gas and oxygen pass through waste gas delivery pipeline road respectively and oxygen bottle enter in gas buffer tank carry out mixing buffering after with a constant current
It measures while being passed through in the first reactor being continuously arranged, second reactor and third reactor and carry out catalysis burning, catalysis burning
The tail gas of processing enters tail gas collecting device, is discharged after adsorption treatment by exhaust outlet；It is arranged in the first reaction response device
The second catalyst bed is arranged in the second reactor for first catalyst bed, and setting third is urged in the third reactor
Agent bed.The temperature of first reactor controls between 100-200 DEG C, and the temperature of second reactor is controlled at 200-300 DEG C
Between, the temperature of third reactor controls between 300-400 DEG C.
The catalyst that first catalyst bed loads are as follows: using active carbon as carrier, LaO2For active component, alkali metal
For auxiliary agent；Wherein, LaO2The 6-15% of catalyst weight is accounted for, alkali metal accounts for the 0.1%~2% of catalyst weight, and surplus is to live
Property charcoal；The alkali metal is one or more of Li, Na, K, Ru, Cs.
Complex rare-earth oxidate containing valuable metal, especially LaO2With good storage put oxygen performance and oxygen mobility, to the depth of CVOCs
Aoxidize it is highly beneficial, therefore CVOCs catalysis oxidation field application have received widespread attention.And LaO2With certain acidity
With because of La4+/ La3+Reversible transformation and have good storage put oxygen performance and oxygen mobility.Allow catalyst in air ring
In border, the chloralkanes such as chlorine volatile organic matter methylene chloride will be contained long-term and stably and be converted into H2O、CO2And HCl.
Above-mentioned catalyst is prepared via a method which: a certain amount of soluble lanthanum salt and a certain amount of alkali metal salt are dissolved
In a certain amount of water, then to being added absorbent charcoal carrier in solution, and the mixture is kept stirring 2 hours, it then will mixing
Object is heated to 130 DEG C, and keeps the temperature 24 hours.Solid product, is then dried overnight, finally in height by filtering at 80 DEG C
It is roasted in the lower air of temperature, tabletting, sieving (40-60 mesh) is afterwards to obtain the final product.
The concentration and impregnation ratio for controlling each solution during the preparation process, make resulting catalyst have following characteristics:
LaO2The 6-15% of catalyst weight is accounted for, alkali metal accounts for the 0.1%~2% of catalyst weight, and surplus is active carbon；The high temperature
Roasting refers in 400~600 DEG C of 2~5h of roasting.
The catalyst that second catalyst bed loads are as follows: with TiO2Particle is carrier, with CuO-Co3O4For active group
Point；Wherein, CuO accounts for 6~18%, Co of catalyst weight3O4Account for the 20%~45% of catalyst weight, surplus TiO2Particle.
Using TiO2Particle is carrier, and active component is strong with basal body binding force, not easily to fall off and cracking, in high-speed air-flow and thermal shock
Under be still able to maintain greater activity.Catalyst reaches 95% or more to the conversion ratio of the chlorinated aromatic hydrocarbons such as o-dichlorohenzene at 300 DEG C.
Above-mentioned catalyst is prepared via a method which: by a certain amount of soluble copper salt and a certain amount of salt solubility in one
In gauge water, then to TiO is added in solution2Particle, and the mixture is kept stirring 2 hours, then mixture is heated
To 130 DEG C, and keep the temperature 24 hours.Solid product, is then dried overnight by filtering at 80 DEG C, finally empty at high temperature
It is roasted in gas, tabletting, sieving (40-60 mesh) is afterwards to obtain the final product.
The concentration and impregnation ratio for controlling each solution during the preparation process, make resulting catalyst have following characteristics: CuO
Account for 6~18%, Co of catalyst weight3O4Account for the 20%~45% of catalyst weight, surplus TiO2Particle.
The catalyst that the third catalyst bed loads are as follows: the catalyst includes cerium oxide nano-rod and Metal Palladium, is pressed
Weight calculates, and the content of palladium is 0.5%, remaining is cerium oxide nano-rod.It is used as and is urged using the precious metal palladium with high catalytic activity
Agent active component, especially suitable for when chloralkane content is low in tail gas, chlorinatedorganic and catalysis combustion by-products
Catalyzed conversion.
Above-mentioned catalyst is prepared via a method which: cerous nitrate being mixed with sodium hydroxide solution, is stirred in beaker equal
It is fitted into after even in the crystallizing kettle with polytetrafluoroethyllining lining, after a certain period of time, sediment is filtered for crystallization at different temperatures
Drying is washed, 350 DEG C of calcining 3h, obtain the cerium oxide carrier of different-shape in air atmosphere；By soluble palladium saline solution
It is impregnated into cerium oxide carrier powder, is uniformly dispersed, dried after standing, in air atmosphere 400 DEG C of calcining 4h, tabletting, sieving
(40-60 mesh) afterwards to obtain the final product.
The adsorbent that the adsorption treatment uses is granular activated carbon, partial size 2-5mm.
The organic exhaust gas containing chlorine and oxygen is passed through after gas buffer tank is buffered logical with 3.8~6.9L/min flow
Enter reaction column；The oxygen accounts for the 50%-80%(V/V of mixed gas total amount).
What the compare with the existing technology present invention had has the technical effect that
(1) be directed to CVOCs tail gas complicated composition the case where, by be continuously arranged first reactor, second reactor and
Third reactor avoids single-reactor from not being suitable for multi-component CVOCs catalysis burning bring emission not up to standard
Technical problem, wherein the catalyst bed of first reactor uses LaO2/ active carbon allows catalyst to exist as catalyst
In air environment, it will pointedly contain the chloralkanes such as chlorine volatile organic matter methylene chloride long-term and stably and be converted into H2O、
CO2And HCl.For chlorinated aromatic hydrocarbons component, the catalyst layer for the second reactor being arranged in reaction column uses TiO2Particle is to carry
Body, active component is strong with basal body binding force, and not easily to fall off and cracking is still able to maintain higher work under high-speed air-flow and thermal shock
Property.Catalyst reaches 95% or more to the conversion ratio of the chlorinated aromatic hydrocarbons such as o-dichlorohenzene at 300 DEG C.The catalyst bed of third reactor
Layer, using palladium/nano-cerium oxide stick as catalyst activity component, especially suitable for when chloralkane content is low in tail gas, chlorine
For organic matter and the catalyzed conversion of catalysis combustion by-products.
(2) present invention process is simple, and the catalyst activity stable service life is up to 300 hours or more, organochlorine exhaust gas removal efficiency
Up to 99% or more.
Specific embodiment
The following is a clear and complete description of the technical scheme in the embodiments of the invention, it is clear that described embodiment
Only a part of the embodiment of the present invention, instead of all the embodiments.Based on the embodiments of the present invention, the common skill in this field
Art personnel every other embodiment obtained without making creative work belongs to the model that the present invention protects
It encloses.
[embodiment 1]
The preparation of catalyst:
(1) a certain amount of lanthanum nitrate and a certain amount of potassium chloride are dissolved in a certain amount of water, then to being added in solution
Absorbent charcoal carrier, and the mixture is kept stirring 2 hours, 130 DEG C are then heated the mixture to, and keep the temperature 24 small
When.Solid product, is then dried overnight by filtering at 80 DEG C, and 4.5h, tabletting, sieving are finally roasted at 500 DEG C of air atmosphere
(40-60 mesh) is afterwards up to catalyst A.
The concentration and impregnation ratio for controlling each solution during the preparation process make resulting catalyst A have following characteristics:
LaO2The 7.2% of catalyst weight is accounted for, metallic potassium accounts for the 0.8% of catalyst weight, and surplus is active carbon.
(2) copper nitrate and cobalt chloride are dissolved in a certain amount of water, then to TiO is added in solution2Particle, and this is mixed
It closes object to be kept stirring 2 hours, then heats the mixture to 130 DEG C, and keep the temperature 24 hours.Filtering, then by solid
Product is dried overnight at 80 DEG C, 3h is finally roasted at 430 DEG C of air atmosphere, tabletting, sieving (40-60 mesh) is afterwards up to catalyst
B。
The concentration and impregnation ratio for controlling each solution during the preparation process make resulting catalyst B have following characteristics:
CuO accounts for 12%, Co of catalyst weight3O4Account for the 32% of catalyst weight, surplus TiO2Particle.
(3) cerous nitrate is mixed with sodium hydroxide solution, is packed into after mixing evenly in beaker in polytetrafluoroethylene (PTFE)
In the crystallizing kettle of lining, crystallization is after a certain period of time, dry by sediment filtration washing at different temperatures, and in air atmosphere 350
DEG C calcining 3h, obtain the cerium oxide carrier of different-shape；Soluble palladium saline solution is impregnated into cerium oxide carrier powder, point
It dissipates uniformly, is dried after standing, in air atmosphere 400 DEG C of calcining 4h, tabletting, sieving (40-60 mesh) is afterwards up to catalyst C.?
The concentration and impregnation ratio that each solution is controlled in preparation process make resulting catalyst B have following characteristics: calculating by weight,
The content of palladium is 0.5%.
VOCs treatment containing chlorine:
The organic exhaust gas containing chlorine of certain chemical plant emission: chloromethanes 500ppm, methylene chloride 1200ppm, vinyl chloride 90ppm,
Chlorobenzene 2500ppm, 1,2- dichloroethanes 380ppm.
Above-mentioned organic exhaust gas containing chlorine and oxygen are passed through into waste gas delivery pipeline road respectively and oxygen bottle enters gas buffer tank
In carry out mixing buffering, control the 56%(V/V that the oxygen accounts for mixed gas total amount), be then passed through with 5.2L/min flow
The first reaction column, the second reaction column and the third reaction column being continuously arranged, the reaction column are 55m reaction column, the first reaction
Column loading catalyst A, the second reaction column loading catalyst B, third reaction column loading catalyst C, the first reaction column temperature control
At 175 DEG C, at 300 DEG C, the temperature of third reaction column is controlled at 370 DEG C for the temperature control of the second reaction column.It is catalyzed burning processing
Tail gas enter tail gas collecting device, be discharged after adsorption treatment by exhaust outlet, discharge air-flow detect chlorinated organics content: chlorine
Methane 1.0ppm, methylene chloride 1.1ppm, vinyl chloride 0ppm, chlorobenzene 1.1ppm, 1,2- dichloroethanes 0.4ppm.It is computed, it is main
Want the removal efficiency of chlorinated organics 99.8% or more.
Continuous operation is tested after 330 hours, emission chlorinated organics content: chloromethanes 2.2ppm, methylene chloride
3.1ppm, vinyl chloride 0.2ppm, chlorobenzene 2.2ppm, 1,2- dichloroethanes 3.2ppm.It is computed, main chlorinated organics take off
Except rate is 99.2% or more.
[embodiment 2]
The organic exhaust gas containing chlorine of certain chemical plant emission: chloromethanes 500ppm, methylene chloride 1200ppm, vinyl chloride 90ppm,
Chlorobenzene 2500ppm, 1,2- dichloroethanes 380ppm.
Above-mentioned organic exhaust gas containing chlorine and oxygen are passed through into waste gas delivery pipeline road respectively and oxygen bottle enters gas buffer tank
In carry out mixing buffering, control the 56%(V/V that the oxygen accounts for mixed gas total amount), be then passed through with 4.4L/min flow
The first reaction column, the second reaction column and the third reaction column being continuously arranged, the reaction column are 55m reaction column, the first reaction
Column loading catalyst A, the second reaction column loading catalyst B, third reaction column loading catalyst C, the first reaction column temperature control
At 120 DEG C, at 210 DEG C, the temperature of third reaction column is controlled at 350 DEG C for the temperature control of the second reaction column.It is catalyzed burning processing
Tail gas enter tail gas collecting device, be discharged after adsorption treatment by exhaust outlet, discharge air-flow detect chlorinated organics content: chlorine
Methane 1.5ppm, methylene chloride 2.3ppm, vinyl chloride 0.4ppm, chlorobenzene 1.2ppm, 1,2- dichloroethanes 0.2ppm.It is computed,
The removing of main chlorinated organics is 99.7% or more.
Continuous operation is tested after 500 hours, emission chlorinated organics content: chloromethanes 2.2ppm, methylene chloride
4.3ppm, vinyl chloride 0.5ppm, chlorobenzene 2.2ppm, 1,2- dichloroethanes 3.3ppm.It is computed, main chlorinated organics take off
Except rate is 99.3% or more.
[comparative example 1]
VOCs treatment containing chlorine:
The organic exhaust gas containing chlorine of certain chemical plant emission: chloromethanes 500ppm, methylene chloride 1200ppm, vinyl chloride 90ppm,
Chlorobenzene 2500ppm, 1,2- dichloroethanes 380ppm.
Above-mentioned organic exhaust gas containing chlorine and oxygen are passed through into waste gas delivery pipeline road respectively and oxygen bottle enters gas buffer tank
In carry out mixing buffering, control the 56%(V/V that the oxygen accounts for mixed gas total amount), be then passed through with 5.2L/min flow
The first reaction column, the second reaction column and the third reaction column being continuously arranged, the reaction column are 55m reaction column, three reactions
The equal loading catalyst A of column, the first reaction column temperature control is at 175 DEG C, and the temperature of the second reaction column is controlled at 300 DEG C, and third is anti-
The temperature of Ying Zhu is controlled at 370 DEG C.The tail gas of catalysis burning processing enters tail gas collecting device, by exhaust outlet after adsorption treatment
Discharge, discharge air-flow detect chlorinated organics content: chloromethanes 1.7ppm, methylene chloride 0.2ppm, vinyl chloride 1.1ppm, chlorobenzene
456ppm, 1,2- dichloroethanes 8.5ppm.It is computed, the removal efficiency of chlorobenzene is only 81.3%.
[comparative example 2]
VOCs treatment containing chlorine:
The organic exhaust gas containing chlorine of certain chemical plant emission: chloromethanes 500ppm, methylene chloride 1200ppm, vinyl chloride 90ppm,
Chlorobenzene 2500ppm, 1,2- dichloroethanes 380ppm.
Above-mentioned organic exhaust gas containing chlorine and oxygen are passed through into waste gas delivery pipeline road respectively and oxygen bottle enters gas buffer tank
In carry out mixing buffering, control the 56%(V/V that the oxygen accounts for mixed gas total amount), be then passed through with 5.2L/min flow
The first reaction column, the second reaction column and the third reaction column being continuously arranged, the reaction column are 55m reaction column, three reactions
Column loading catalyst B, the first reaction column temperature control is at 175 DEG C, and at 300 DEG C, third is reacted for the temperature control of the second reaction column
The temperature of column is controlled at 370 DEG C.The tail gas of catalysis burning processing enters tail gas collecting device, is arranged after adsorption treatment by exhaust outlet
Out, discharge air-flow detects chlorinated organics content: chloromethanes 15ppm, methylene chloride 152ppm, vinyl chloride 3.5ppm, chlorobenzene
0.3ppm, 1,2- dichloroethanes 0.7ppm.It is computed, the removal efficiency of methylene chloride is only 87.3%.
[comparative example 3]
VOCs treatment containing chlorine:
The organic exhaust gas containing chlorine of certain chemical plant emission: chloromethanes 500ppm, methylene chloride 1200ppm, vinyl chloride 90ppm,
Chlorobenzene 2500ppm, 1,2- dichloroethanes 380ppm.
Above-mentioned organic exhaust gas containing chlorine and oxygen are passed through into waste gas delivery pipeline road respectively and oxygen bottle enters gas buffer tank
In carry out mixing buffering, control the 56%(V/V that the oxygen accounts for mixed gas total amount), be then passed through with 5.2L/min flow
The first reaction column, the second reaction column and the third reaction column being continuously arranged, the reaction column are 55m reaction column, three reactions
The equal loading catalyst C of column, the first reaction column temperature control is at 175 DEG C, and the temperature of the second reaction column is controlled at 300 DEG C, and third is anti-
The temperature of Ying Zhu is controlled at 370 DEG C.The tail gas of catalysis burning processing enters tail gas collecting device, by exhaust outlet after adsorption treatment
Discharge, discharge air-flow detect chlorinated organics content: chloromethanes 0ppm, methylene chloride 0ppm, vinyl chloride 0ppm, chlorobenzene 0ppm,
1,2- dichloroethanes 0.1ppm.It is computed, the removal efficiencies of main chlorinated organics is close to 100%.
Continuous operation is tested after 30 hours, emission chlorinated organics content: chloromethanes 35ppm, methylene chloride
56ppm, vinyl chloride 18ppm, chlorobenzene 102ppm, 1,2- dichloroethanes 45ppm.It is computed, the removal efficiency of main chlorinated organics
Only 88% or so.
It can be seen that the present invention is successively loaded by the way that first reactor, second reactor and third reactor is continuously arranged
Catalyst A with given activity, catalyst B and catalyst C, solve single reaction column be not suitable for it is multi-component
CVOCs catalysis burning bring emission technical problem not up to standard, the removal efficiency of the organic exhaust gas containing chlorine reach 99% or more；
The service life of catalyst is additionally extended, remains within continuous operation 300 hours or more obtain satisfied removal efficiency, contain compared to traditional
Chlorine organic exhaust gas removing process has incomparable advantage.
Above description sufficiently discloses a specific embodiment of the invention.It should be pointed out that being familiar with the field
Range of any change that technical staff does a specific embodiment of the invention all without departing from claims of the present invention.
Correspondingly, the scope of the claims of the invention is also not limited only to previous embodiment.
Claims (3)
1. a kind of processing method for the organic exhaust gas containing chlorine, it is characterised in that: chlorine organic exhaust gas will be contained and oxygen passes through respectively
Waste gas delivery pipeline road and oxygen bottle enter in gas buffer tank carry out mixing buffering after continuously set with certain flow while being passed through
Catalysis burning is carried out in first reactor, second reactor and the third reactor set, the tail gas of catalysis burning processing enters tail
Gas collection device, is discharged after adsorption treatment by exhaust outlet；First catalyst bed is set in the first reactor, described
Second catalyst bed is set in two reactors, third catalyst bed is set in the third reactor；First reactor
Temperature controls between 100-200 DEG C, and the temperature of second reactor controls the temperature of third reactor between 200-300 DEG C
Control is between 300-400 DEG C；The catalyst that first catalyst bed loads are as follows: using active carbon as carrier, LaO2 is to live
Property component, alkali metal is auxiliary agent；Wherein, LaO2 accounts for the 6-15% of catalyst weight, alkali metal account for catalyst weight 0.1%~
2%, surplus is active carbon；The alkali metal is one or more of Li, Na, K, Cs；Second catalyst bed loads
Catalyst are as follows: using TiO2 particle as carrier, using CuO-Co3O4 as active component；Wherein, CuO account for catalyst weight 6~
18%, Co3O4 account for the 20%~45% of catalyst weight, and surplus is TiO2 particle；What the third catalyst bed loaded urges
Agent are as follows: the catalyst includes cerium oxide nano-rod and Metal Palladium, is calculated by weight, and the content of palladium is 0.5%, remaining is oxidation
Cerium nanometer rods.
2. the processing method according to claim 1 for the organic exhaust gas containing chlorine, which is characterized in that the adsorption treatment
The adsorbent used is granular activated carbon, partial size 2-5mm.
3. the processing method according to claim 1 for the organic exhaust gas containing chlorine, which is characterized in that described is organic containing chlorine
Exhaust gas and oxygen are passed through after gas buffer tank is buffered and are passed through reactor with 3.8~6.9L/min flow；The oxygen accounts for
The 50%-80%(V/V of mixed gas total amount).
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