CN108114570A - One kind contains CS for handling2And H2The method of S mixed pollutants exhaust gas - Google Patents

One kind contains CS for handling2And H2The method of S mixed pollutants exhaust gas Download PDF

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CN108114570A
CN108114570A CN201710236095.0A CN201710236095A CN108114570A CN 108114570 A CN108114570 A CN 108114570A CN 201710236095 A CN201710236095 A CN 201710236095A CN 108114570 A CN108114570 A CN 108114570A
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exhaust gas
adsorption
temperature plasma
handling
low temperature
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CN108114570B (en
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龙超
刘笑寒
马佳凯
刘慧娟
张健
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Nanjing University
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Nanjing University
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
    • B01D53/1456—Removing acid components
    • B01D53/1468—Removing hydrogen sulfide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
    • B01D53/1487—Removing organic compounds
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
    • B01D53/323—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00 by electrostatic effects or by high-voltage electric fields
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
    • B01D2252/10—Inorganic absorbents
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2253/00—Adsorbents used in seperation treatment of gases and vapours
    • B01D2253/20—Organic adsorbents
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2259/00—Type of treatment
    • B01D2259/80—Employing electric, magnetic, electromagnetic or wave energy, or particle radiation
    • B01D2259/818—Employing electrical discharges or the generation of a plasma

Abstract

Contain CS the invention discloses one kind for handling2And H2The method of S mixed pollutants exhaust gas, belongs to technical field of waste gas treatment.The present invention contains CS for what is discharged during the industry productions such as synthetic fibers, leather, pharmacy2And with a small amount of H2The exhaust gas of S discloses a kind of method handled using absorption low temperature plasma oxidation absorption integrated technique, and super high cross-linked adsorbing resin is to CS2With high selective adsorption capacity, recyclable more than 99% CS2, avoid the wasting of resources；Low temperature plasma can be efficiently by a small amount of H2S and CS2It is oxidized to CO2, H2O and SO2, completely eliminate the foul odour of exhaust gas, SO in tail gas2It is absorbed using lye, so as to fulfill H2S、CS2And SO2Complete qualified discharge.

Description

One kind contains CS for handling2And H2The method of S mixed pollutants exhaust gas
Technical field
The invention belongs to exhaust-gas treatment fields, and in particular to be generated during to industry productions such as synthetic fibers, pharmacy Containing CS2And H2The processing method of S exhaust gas, more specifically to a kind of adsorption-low temperature plasma oxidation-absorption integrated technique Processing is containing CS2And H2The method of S exhaust gas.
Background technology
In the production process of the industries such as synthetic fibers, leather, pharmacy, often generate and largely contain CS2And with a small amount of H2The exhaust gas of S, the two are the low odorant of threshold value, and can generate damage to the smell of human body and nervous system, therefore It is very necessary and urgent effectively to administer such exhaust gas.For such tail gas, existing processing method all there are it is certain the defects of. Such as Crouse's oxidizing process, principle is to make sulfide imperfect combustion, and element sulphur is made to be converted into elemental sulfur.The technique is for exhaust gas Pressure there are certain requirements, while the technique handles CS in a manner of aoxidizing2, while wasting resource, SO can be generated2By-product, Easily cause secondary pollution.For another example alkali absorption method, using lye (such as NaOH or NaHCO3) with more efficient can absorb in exhaust gas H2S is simultaneously converted into the solid products such as NaHS, but lye is for CS2Absorption efficiency it is relatively low.
Such as the publication CN104474875A (times of disclosure：On 04 01st, 2015) disclose a kind of H2S and CS2Mixing The absorption technique of gas.The technique is passed through air heating until going out by lye spray-absorption exhaust gas, and by the solution after neutralization Existing simple substance S precipitations continue to be heated to precipitation dissolving, generate sodium polysulfide, and S elements can be fixed as Zhu by input Hg simple substance reactions Sand (HgS).The for another example 102743969 A (times of disclosure of publication CN：On October 24th, 2012) disclose a kind of absorption-suction Attached technical finesse contains H2S and CS2The processing method of exhaust gas.Technology utilization NaHCO3Solution absorbs the H in exhaust gas2S, and point From obtaining NaHS；Tail gas is passed through adsorption recovery CS in the adsorption tower containing granular activated carbon again2, it is achieved thereby that containing CS2With H2The improvement of S mixed pollutants exhaust gas.But there are some drawbacks for the invention：H in tail gas still containing below 10ppm2S is higher than The discharge value (0.05ppm, GB14554-93) of national standard；Contain the moisture close to saturation in the exhaust gas absorbed by lye, Consequent activities charcoal can be significantly reduced to CS2Adsorption efficiency (bibliography：Fan Huiling etc., activated carbon and fixed bed pair under aqueous vapor atmosphere The adsorption dynamics adsorption kinetics behavior of carbon disulfide, ACTA Scientiae Circumstantiae, 1999,5 (9), 489-493)；Moreover, after vapor parsing Activated carbon needs drying, cool processing, and otherwise the moisture of activated carbon adsorption can also reduce next cycle to CS2Absorption, but This extends processing technological flow, increases operating cost.In addition, the H not absorbed by lye2S, can be under activated carbon catalysis effect Simple substance S is oxidized to, so that activated carbon blocks (bibliography：Wu Lang, with activated carbon removing low concentration H2The research of S gases, Dalian University of Technology's master thesis, 2005).
Lower temperature plasma technology is to generate high energy electron isoreactivity component using high voltage, contaminant molecule is carried out thorough Bottom oxidative degradation has the characteristics that processing is thorough, simple for process, reaction speed is fast.Low temperature plasma and adsorbing coupled technology It is widely used in the removal of VOCs, still, usually adsorbent is filled in inside reaction of low temperature plasma device with reinforcing etc. Gas ions regenerate the adsorbent of adsorption saturation to the degradation of VOCs or using low temperature plasma, can not all realize The recycling of useful resources.
The content of the invention
1. it to solve the problems, such as
Contain H for existing lye absorption-active carbon adsorption technology processing2S and CS2Shortcomings present in exhaust gas, such as alkali Liquid removes H2S efficiency is low, H2S is oxidized to elemental sulfur by activated carbon catalysis and causes adsorbent bed blocking, moisture that activated carbon is caused to remove energy H in power and mechanical strength decline and tail gas2S and CS2It is difficult to up to standard etc., the present invention proposes a kind of hypercrosslinked polymeric resin and inhales The integrated new process that attached-low-temperature plasma degradation-lye absorbs, can improve to CS2Organic efficiency and H2The removal efficiency of S, Realize CS2High efficiente callback and H2S and CS2Stably reaching standard discharges.The present invention not only solves exhaust emission as topic, and realizes The recycling of useful resources.
2. technical solution
To solve the above-mentioned problems, the technical solution adopted in the present invention is as follows：
One kind contains CS for handling2And H2The process system of S mix waste gas, including sequentially connected adsorption tower, low temperature etc. Gas ions processing unit and lye absorption tower, the bottom of the adsorption tower set gas inlet end, top set vapor into Enter end, polystyrene super high cross-linked adsorbing resin is filled in adsorption tower；The electric discharge of the reaction of low temperature plasma device Mode is dielectric barrier discharge, corona discharge or creeping discharge.
Further, there are two the adsorption towers, one is set between adsorption tower and apparatus for low-temperature plasma treatment Grade condenser and secondary condenser, for being condensed to absorption regeneration steam.
One kind contains CS for handling2And H2The method of S mixed pollutants exhaust gas, using above-mentioned hypercrosslinked polymeric resin absorption- Low temperature plasma oxidation-lye absorbs integrated technique and is handled, and specific steps include：
(1) CS will be contained2And H2The adsorption tower that the exhaust gas introducing of S is filled with absorption resin carries out adsorption treatment, selective absorption Recycle CS in exhaust gas2；It is polystyrene super high cross-linked adsorbing resin wherein to adsorb resin, and specific surface area is more than 900m2/ g, Micropore volume is more than 0.3mL/g and micropore size is distributed between 0.5-1.0nm.
(2) exhaust gas crossed through adsorption treatment is passed through reaction of low temperature plasma device, for removing H2S and minute quantity not by The CS of sorbing material absorption2, effectively by H2S and CS2It is degraded to CO2, H2O and SO2, H2S and CS2Concentration reaches country's discharge mark It is accurate；
(3) lye absorption tower will be passed through through the processed exhaust gas of reaction of low temperature plasma device, absorbs low temperature plasma Oxidative degradation H2By-product SO caused by S2, make SO2Qualified discharge.
Further, in the step (1) adsorption tower altogether there are two, adsorption and desorption process on two towers alternately, One of adsorption tower is in absorption CS2Meanwhile another adsorption tower is desorbed using 100-130 DEG C of vapor, desorption steams Gas is condensed recyclable to obtain CS2, the switching of the adsorption and desorption process of two adsorption towers automatically controlled by PLC program.
Further, the discharge mode of the reaction of low temperature plasma device in the step (2) for dielectric barrier discharge, Corona discharge or creeping discharge etc., apply between two electrodes voltage be 10-25kV, the adjustable high-voltage electricity that frequency is 10-20MHz.
Further, the Alkali absorption liquid in the step (3) can be NaOH, NaHCO3、Na2CO3、K2CO3、KOH、Ca (OH)2One or more combinations therein, solution concentration is generally in 5wt%-20wt%.
3. advantageous effect
Compared with the prior art, beneficial effects of the present invention are：
(1) sorbing material of the invention is using polystyrene super high cross-linked adsorbing resin, and surface is high hydrophobicity, moisture Son with absorption resin intermolecular forces it is extremely weak, thus in exhaust gas moisture to CS2Absorption do not influence, to CS in humid gas2It protects Hold high adsorption capacity；Due to surface hydrophobic, after absorption resin is using vapor desorption, processing need not be dried, letter Change technical process, reduce energy consumption；Moreover, the micropore size of absorption resin is distributed in 0.5-1.0nm, it is wide in range compared to aperture The super high cross-linked adsorbing resin of distribution is substantially increased to high volatile CS2Adsorption capacity；
(2) sorbing material of the invention is high molecular polymer, is not had using polystyrene super high cross-linked adsorbing resin Catalysis, thus H2When S gases pass through adsorption bed, it will not be elemental sulfur by catalysis oxidation, avoid activated carbon adsorption The problem of elemental sulfur blocks in journey；
(3) " hypercrosslinked polymeric resin adsorption-low temperature plasma oxidation-lye absorbs " process H of the invention2S and CS2Mixed pollutants exhaust gas, recyclable more than 95% CS2, avoid the wasting of resources, and H2S、CS2And SO2Complete row up to standard It puts；
(4) present invention contains CS for what is discharged during the industry productions such as synthetic fibers, leather, pharmacy2And with a small amount of H2The characteristics of S exhaust gas, it is proposed that the integrated treatment process that hypercrosslinked polymeric resin adsorption-low temperature plasma oxidation-lye absorbs, To realize to CS2Resource reclaim and H2S and CS2The purpose of qualified discharge.
Description of the drawings
Fig. 1 is the structure diagram of the process system of the present invention；
In figure：1st, gas inlet end；2nd, air inducing wind turbine；3rd, emptier；4th, 5- adsorption towers；6th, Low Temperature Plasma Treating Device；7th, lye absorption tower；8th, vapor upstream end；9th, first-stage condenser；10th, secondary condenser；11st, collecting tank.
Specific embodiment
The present invention is further described below with reference to specific embodiment.
Embodiment 1
As shown in Figure 1, a kind of contain CS for handling2And H2The process system of S mix waste gas, including sequentially connected suction Attached tower 4,5, apparatus for low-temperature plasma treatment 6 and lye absorption tower 7, adsorption tower 4 and adsorption tower 5 connect side by side, adsorption and desorption On two towers alternately, the switching of the adsorption and desorption process of two adsorption towers is automatically controlled process by PLC program, adsorption tower 4th, 5 bottom sets gas inlet end 1, air inducing wind turbine 2 and emptier 3, and 4,5 top of adsorption tower sets vapor upstream end 8, Polystyrene super high cross-linked adsorbing resin is filled in adsorption tower 4；Between adsorption tower 4 and apparatus for low-temperature plasma treatment 6 First-stage condenser 9 and secondary condenser 10 are set, collecting tank 11, first-stage condenser 9 and two level are connected on secondary condenser 10 The effect of condenser 10 is that absorption regeneration steam is condensed.
Processing contains CS2And H2The method of S mixed pollutants exhaust gas, including absorption process, Low Temperature Plasma Treating process With desorption process, detailed process is as follows：
1. absorption process
Containing CS2With H2The exhaust gas of S carries out absorption behaviour under the action of air inducing wind turbine 2 from gas inlet end 1 into adsorption tower 4 Make, the CS in selective removal exhaust gas2.When absorption, which reaches, to be penetrated, PLC program control air intake valve is closed, and is transferred to desorption rank Section, while adsorption tower 5 initially enters absorption phase, two adsorption towers carry out adsorption and desorption operation in turn.
2. Low Temperature Plasma Treating process
Gas enters plasma reactor 6, which can be by H2S and a small amount of CS not to be adsorbed2It is oxidized to CO2, H2O and SO2.Purified gas eventually enters into lye absorption tower 7, to remove the SO in tail gas2, so far, exhaust gas obtains thoroughly Processing.
3. it is desorbed process
Vapor carries out desorption manipulation from entrance 8 into adsorption tower upper end to the adsorption tower 4 or 5 of adsorption penetration.Outlet Contain high concentration CS2Steam first pass through first-stage condenser 9 and cool, then by 10 deep condensation of secondary condenser, make CS2 Liquid is condensed into, is collected in collecting tank 11.Contain a small amount of CS2Fixed gas and adsorption tower tail gas import low temperature plasma Reactor carries out advanced treating.
When being in an emergency, emptying operation can be carried out from the evacuated tube 3 of inlet end.
Embodiment 2
Handle CS2With H2The exhaust gas of S mixtures, main parameter have：Air inducing fan delivery 80CMH, CS2Inlet gas concentration 5g/ m3, H2S concentration 1000mg/m3Intake air temperature room temperature, pressure normal pressure；Absorber diameter DN=180mm, adsorbent are superhigh cross-linking Resin NDA-150 resins are adsorbed, load height H=300mm, adsorption time 90min, vapor desorption time 60min, level-one Condenser uses normal temperature circulation water, and secondary condenser uses 5 DEG C of chilled brine；Low temperature plasma uses corona discharge side Formula, voltage 25kV, frequency 20MHz；Absorbing liquid is the NaOH solution of concentration 5wt%.Exhaust gas is after integrated technique is handled, row Put CS in tail gas2With H2S is not detected, and collecting tank recycles CS altogether for 24 hours29.3Kg, the rate of recovery 96.9%.
Embodiment 3
Adsorbent in embodiment 2 is changed to macroporous absorbent resin AMBERLITETMXAD-4, other conditions are constant.Discharge CS in tail gas2Concentration is 103mg/m3, treatment effeciency 97.94%, H2S concentration does not detect.Collecting tank recycles altogether for 24 hours CS26.9Kg, the rate of recovery 71.9%.
Embodiment 4
Low-temperature plasma bulk voltage in embodiment 2 is changed to 10kV, other conditions are constant.CS in emission2Concentration For 42mg/m3, treatment effeciency 99.16%；H2S concentration is 8mg/m3, treatment effeciency 99.2%.
Embodiment 5
Low-temperature plasma bulk voltage in embodiment 2 is changed to 15kV, other conditions are constant.CS in emission2Concentration For 5mg/m3, treatment effeciency 99.9%；H2S is not detected.
Embodiment 6
Low-temperature plasma body frequency in embodiment 2 is changed to 10MHz, other conditions are constant.CS in emission2Concentration For 18mg/m3, treatment effeciency 99.64%, H2S concentration does not detect.
Embodiment 7
Low-temperature plasma body frequency in embodiment 2 is changed to 15MHz, other conditions are constant.CS in emission2Concentration For 6mg/m3, treatment effeciency 99.88%, H2S is not detected.

Claims (9)

1. one kind contains CS for handling2And H2The method of S mixed pollutants exhaust gas, it is characterised in that：Using a kind of superhigh cross-linking Resin adsorption-low temperature plasma oxidation-lye absorbs integrated technique system and is handled, and processing step includes：
(1) CS will be contained2And H2The adsorption tower that the exhaust gas introducing of S is filled with absorption resin carries out adsorption treatment, the absorption resin For polystyrene super high cross-linked adsorbing resin, specific surface area is more than 900m2/ g, Micropore volume are more than 0.3mL/g and micropore Pore-size distribution is between 0.5-1.0nm；
(2) exhaust gas crossed through adsorption treatment is passed through reaction of low temperature plasma device, to H2S and CS not to be adsorbed2It is aoxidized Degradation；
(3) lye absorption tower will be passed through through the processed exhaust gas of reaction of low temperature plasma device, absorbs low temperature plasma oxidation The by-product that degradation generates.
2. one kind according to claim 1 contains CS for handling2And H2The method of S mixed pollutants exhaust gas, feature exist In：The integrated technique system includes sequentially connected adsorption tower (4), apparatus for low-temperature plasma treatment (6) and lye and inhales Tower (7) is received, the bottom of the adsorption tower (4) sets gas inlet end (1), and top sets vapor upstream end (8), adsorption tower (4) polystyrene super high cross-linked adsorbing resin is filled in.
3. one kind according to claim 2 contains CS for handling2And H2The method of S mixed pollutants exhaust gas, feature exist In：There are two the adsorption towers (4), adsorption and desorption process on two towers alternately, the adsorption and desorption mistake of two adsorption towers The switching of journey is automatically controlled by PLC program.
4. one kind according to claim 3 contains CS for handling2And H2The method of S mixed pollutants exhaust gas, feature exist In：First-stage condenser (9) and secondary condenser (10) are further included in integrated technique system, absorption regeneration steam is condensed.
5. one kind according to claim 3 contains CS for handling2And H2The method of S mixed pollutants exhaust gas, feature exist In：Desorption process is recycled after desorption steam is condensed to be desorbed using 100-130 DEG C of vapor and obtains CS2。
6. one kind according to claim 1 or 2 contains CS for handling2And H2The method of S mixed pollutants exhaust gas, it is special Sign is：The discharge mode of reaction of low temperature plasma device described in step (2) is dielectric barrier discharge, corona discharge or edge It discharges in face.
7. one kind according to claim 6 contains CS for handling2And H2The method of S mixed pollutants exhaust gas, feature exist In：Between two electrodes of reaction of low temperature plasma device apply voltage be 10-25kV, the adjustable high pressure that frequency is 10-20MHz Electricity.
8. one kind according to claim 3 or 5 contains CS for handling2And H2The method of S mixed pollutants exhaust gas, it is special Sign is：Alkali absorption liquid in step (3) is NaOH, NaHCO3、Na2CO3、K2CO3、KOH、Ca(OH)2It is therein a kind of or more Kind combination.
9. one kind according to claim 8 contains CS for handling2And H2The method of S mixed pollutants exhaust gas, feature exist In：The concentration of Alkali absorption liquid is 5wt%-20wt%.
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CN112642273A (en) * 2020-12-18 2021-04-13 阿拉尔市中泰纺织科技有限公司 Incineration recovery system and process for converting low-concentration waste gas into high-concentration waste gas through degassing

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