CN107744715A - A kind of flue gas treating process of liquid phase simultaneous SO_2 and NO removal - Google Patents
A kind of flue gas treating process of liquid phase simultaneous SO_2 and NO removal Download PDFInfo
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- CN107744715A CN107744715A CN201711023106.3A CN201711023106A CN107744715A CN 107744715 A CN107744715 A CN 107744715A CN 201711023106 A CN201711023106 A CN 201711023106A CN 107744715 A CN107744715 A CN 107744715A
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- flue gas
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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
- B01D53/14—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
- B01D53/1481—Removing sulfur dioxide or sulfur trioxide
-
- 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
- B01D53/1406—Multiple stage absorption
-
- 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
- B01D53/1418—Recovery of products
-
- 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
-
- 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
- B01D53/1493—Selection of liquid materials for use as absorbents
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- 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
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/40—Nitrogen compounds
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/02—Other waste gases
- B01D2258/0283—Flue gases
Abstract
The invention discloses a kind of method of liquid phase simultaneous SO_2 and NO removal, category flue-gas processing technique field, for solves the problems, such as during the ammonia process of desulfurization caused largely ammonium sulfites can not directly utilize and flue gas in nitrogen oxides.Lyosoption of this method using the primary product ammonium sulfite during the ammonia process of desulfurization as NO, concentration is in the range of 0.01mol/L~0.1mol/L, and add 0.1%~2% surfactant, the pH value of absorbing liquid is 7.5 ± 1, using Bubbling method and sulfur dioxide and nitrogen oxides in absorbefacient CuO absorption from flue gas are added, solves the problems, such as that NO is insoluble in water.The sulfur dioxide removal rate of the method for liquid phase simultaneous SO_2 and NO removal of the present invention is able to maintain that 100%, the removal efficiency of nitrogen oxides can reach more than 73%, desulphurization denitration product is available, and equipment is simple, and operating cost is low, under equal removal efficiency, investment cost is greatly reduced, suitable for big, in, the fume treatment in miniature coal power plant, there is good prospect.
Description
Technical field
The present invention relates to a kind of flue gas treating process of liquid phase simultaneous SO_2 and NO removal, strengthen in particular with bubble techniques
The treatment effect of flue gas, category flue-gas processing technique field.
Background technology
In recent years, as industrialization is fast-developing, the negative effect of atmosphere pollution environmental problem is more and more significant.Wherein cause
Serious environmental problem is NOx caused by fire coal and SO2, controls the method for nitrogen oxides and includes SCR
(SCR), selective catalytic oxidation (SCO) and SNCR (SNCR), but these methods have cost high or
The shortcomings that selectivity is low, is not suitable for promoting the use of on a large scale.For sulfur removal technology, wet desulphurization accounts for the 85% of market proportion
Left and right, wherein again based on calcium method desulfurization.It is more effectively, stable although calcium method flue gas desulfurization has been widely used in industry
Developed rapidly with the ammonia sulfur removal technology of maturation.And ammonium sulfite easily divides as the primary product during the ammonia process of desulfurization
Solution oxidation, hinder its further application.Can be seen that nitric oxide from the feedback data of actual ammonia sweetening process can be with
Ammonium sulfite reacts, and generation can be used as the ammonium sulfate of agricultural fertilizer.However, it is insoluble due to NO, it is anti-in ammonia sweetening process
It should be difficult to remove nitrogen oxides simultaneously.The technology for there be not comparative maturity still at present can realize wet method simultaneous SO_2 and NO removal.
By the use of sodium chlorite and additive as liquid absorbent in patent CN1843574A (2006), and design corresponding
Spouting induction flotation can realize a certain degree of nitric oxide and sulfur dioxide removal rate, suitable for large, medium and small type pot
Stove and other obsolete equipments.
Patent CN104190223A (2014) realizes absorption tower then by improving the equipment of liquid phase oxidation flue gas desulfurization and denitrification
Flow field optimizes, and the superior and the subordinate's slurries separation is more thorough, and investment cost and running cost are greatly reduced under equal eliminating efficiency
With especially suitable for occasions such as glass kilns.
Comparatively, liquid phase oxidation is better than gas phase and catalytic oxidation, but the effect of absorbing liquid is never convex
Show and, and large-scale coal-fired power plant's smoke gas treatment industry is difficult to apply to current technology.
The content of the invention
Present invention aims at provide a kind of denitrating flue gas desulfuration efficiency is high, construction cost and operating cost are low, product can
The wet method simultaneous SO_2 and NO removal method utilized.
Present invention solves the technical problem that solve by the following technical programs:
A kind of flue gas treating process of liquid phase simultaneous SO_2 and NO removal, using the absorbing liquid inside bubbling reactor dedusting
The direct sorption enhanced of nitrogen oxides and sulfur dioxide in flue gas, desulphurization denitration while realizing flue gas.
Comprise the following steps that:
After flue gas dedusting;
Ammonia spirit is prepared, and adds surfactant;
Flue gas after dedusting is passed through ammonia spirit, carries out pre- sweetening process, produces ammonium sulfite as absorbing liquid;
Absorbefacient is added in absorbing liquid, while carries out desulphurization denitration process;
Waste liquid carries out product recovery after out of stock to desulfurization, completes flue gas treatment.
Further, absorbent solution is made up of ammonium sulfite, absorbefacient and additive, wherein the concentration of ammonium sulfite
For 0.01mol/L~1mol/L, the pH of absorbing liquid is 7.5 ± 1;Absorbefacient is CuO, dosage 0.1g/L;Additive is first
Alcohol, ethanol and ethylene glycol, concentration is 0.1%~2%.
Above-mentioned liquid phase simultaneous SO_2 and NO removal method, the preparation method of absorbing liquid are as follows:Prepared in ammoniacal liquor reserve pool
0.01mol/L~1mol/L ammonia spirits, put gas washing pond into, add absorbefacient;And the flue gas after dedusting is passed through gas washing pond
In, flue gas is passed through, ammonium sulfite concentration is reached 0.01mol/L~1mol/L;It is by the flue gas after dedusting now
Desulphurization denitration process can be carried out simultaneously, the effect of ammonia is the acid-base value for maintaining absorbing liquid without departing from claimed range.
Above-mentioned liquid phase simultaneous SO_2 and NO removal method, absorption technique increases ammonium sulfite recovery and step for regeneration afterwards, described
The absorbing liquid for participating in absorption and 5% ammoniacal liquor reaction generation ammonium sulfate, therebetween cooling down are made ammonium sulfate by Product recycling process
Crystallization separates out, and forms ammonium sulfate solid product, and caused mother liquor absorbs gas washing pond by circulation pumped back, recycles.
Above-mentioned liquid phase simultaneous SO_2 and NO removal method, absorption technique increases absorbefacient recycling process afterwards, described
After absorbefacient filtering, after washing can direct plunge into gas washing pond is continuing with.
The present invention has remarkable advantage as follows compared with prior art:
1st, the present invention is to fill absorbing liquid in bubble absorption device, and the absorbing liquid is in the bar that flue-gas temperature is 20~150 DEG C
The sulfur dioxide and nitrogen oxides in flue gas are absorbed under part, therefore simultaneous SO_2 and NO removal can be accomplished.
2nd, the present invention is 1.0~3.0 seconds in gas-liquid contact time, and sulfur dioxide concentration is 0~2000ppm, NO concentration
For 0~1000ppm when, the removal efficiency of sulfur dioxide maintains 100% or so, and it is left that the removal efficiency of nitrogen oxides maintains 73%
The right side, the utilization rate of absorbent maintain 98% or so.
3rd, the present invention has eliminating efficiency high, and investment is low with operating cost expense, and equipment is simple, stable, absorbent
Utilization rate is high, and absorbefacient is renewable, and product is disposable, it is easy to utilize the features such as.
4th, the present invention is not only suitable for the fume treatment of large-scale coal electricity industry, at the same suitable for it is various it is middle-size and small-size using fire coal as
The equipment of main energy sources supply, has extraordinary application prospect.
Brief description of the drawings
Fig. 1 is ammonium sulfite simultaneous SO_2 and NO removal test device schematic diagram of the present invention;
Fig. 2 is the SEM figures of CuO absorbefacients prepared by direct oxidation method of the present invention;
Fig. 3 is the SEM figures of CuO absorbefacients prepared by the precipitation method of the present invention;
Fig. 4 tests simultaneous SO_2 and NO removal results of property figure, 0.05M ammonium sulfites (NS) for the present invention;1% surfactant
(S);0.1gCuO(C1:Direct oxidation method, C2:The precipitation method);Lucifuge condition (dark);
Fig. 5 is present invention test simultaneous SO_2 and NO removal pollution gas (N2O) selective result figure, 0.05M ammonium sulfites
(NS);1% surfactant (S);0.1gCuO(C1:Direct oxidation method, C2:The precipitation method);Lucifuge condition (dark);
Fig. 6 is the results of property and N that the present invention tests simultaneous SO_2 and NO removal under the conditions of the co-catalyst of various dose2O
Selective result figure;
Fig. 7 is the concrete operations process schematic representation of the present invention.
Embodiment
With reference to embodiment, the present invention is further elaborated.
The present invention be in bubbling reactor, flue gas blasted by dust arrester produced in absorbing liquid it is substantial amounts of tiny
Bubble, in bubble uphill process, mass-transfer progress is completed, reaches gas cleaning purpose.Poured into bubbling reactor
The absorbing liquid of certain liquid level, the titanium dioxide under conditions of the absorbing liquid is 20~150 DEG C in flue-gas temperature in absorption flue gas
Sulphur S02(concentration 0-2000mg/L) and nitrogen oxide NOx (concentration 0-1000mg/L);Absorbing liquid processing dress after the reaction
In putting, the ammonium sulfate in absorbing liquid is formed into supersaturated solution with ammoniacal liquor, then crystallisation by cooling is converted into sulfuric acid by precipitation, produces
Mother liquor by circulate pumped back bubble absorption reaction unit recycle, be filtrated to get CuO washing after can reuse.
Absorbing liquid is 0.01nol/L~1mol/L ammonium sulfite solution, and adds the 0.1%~2% of absorbing liquid volume
Additive, the pH value of absorbing liquid is 6~8, and the additive is one kind or its combination in ethanol, methanol and ethylene glycol.Inhale
Receive agent and the nitrogen oxide NOx reaction generation ammonium sulfate in sulfur dioxide reaction the generation ammonium sulfite, with flue gas in flue gas.
So as to remove sulfureous in flue gas and nitrogen, its main chemical reactions is as follows:
NO+HSO3 -N2O+SO4 2-+H+;
NO+SO3 2-[(NO)SO3]2-;
In the present invention, ammonium sulfite needs to maintain under certain acid-base value condition and the facilitation of additive to two
The absorption efficiency of sulfur oxide and nitrogen oxides is higher, and the utilization rate of ammonium sulfite can also increase therewith.The addition of surfactant,
Gas liquid interfacial area can be greatly improved, increase the probability of flesh absorbing liquid and gas reaction, absorbed so as to drastically increase to nitrogen oxygen
The absorption of compound and sulfur dioxide.
The preparation method of absorbing liquid is:Ammonium sulfite solution, absorbefacient is made by proportioning in absorbing liquid preparation tank and adds
Add the mixed solution of agent, between the acid-base value of absorbing liquid is maintained into 6~8 by ammoniacal liquor, temperature control is between 20~60 DEG C.
Participate in reacted absorbing liquid crystallisation by cooling in product recoverer and generate ammonium sulfate.Reclaim and fill in absorption product
In putting, cooled down indirectly with mechanical agitation, and water, separate out ammonium sulfate crystallization, form ammonium sulfate solid product, caused mother liquor
Absorbing liquid preparing device is sent back to by circulation fluid, recycled.Renewable profit after absorbefacient is washed after filtering with clear water
With without other processing.
It is of the present invention to be advantageous for promoting ammonium sulfite to sulphur, the device of nox adsorption.In bubble absorption
In reactor when gas is sprayed onto in liquid with certain speed and pressure, the bubble of floating can be due to surfactant formed body
Product very little, drastically being disperseed to form JBR layer, bubble produces eddy motion, and the fluid vortex for having interior circulation acts on, from
And increase mass transfer area, absorbing liquid is fully contacted absorption with the sulphur in flue gas and nitrogen.The air that reactor is blasted by air pump passes through
It is uniformly distributed by gas distribution grid in reactor, and turbulization, increase gas liquid interfacial area, promote sulphur and nitrogen oxide
Oxidative absorption, and may advantageously facilitate the further oxidation of ammonium sulfite.
Concrete operations of the present invention are as follows:As shown in fig. 7, the ammoniacal liquor prepared it is isometric be passed through one-level, two level gas washing pond,
Proportionally add absorbefacient;Flue gas passes through dust arrester dedusting, and the flue gas after purifying sequentially enters two level gas washing
Pond, one-level gas washing pond;In the process, the sulfur dioxide in flue gas and ammoniacal liquor reaction generation ammonium sulfite;When in gas washing pond
The acid-base value of the solution in face maintains 7.5 ± 1, and flue gas starts simultaneous SO_2 and NO removal process, and nitrogen oxides can quilt in flue gas
Solution absorbs;The filtrate in one-level gas washing pond enters two level gas washing pond, and the filtrate in two level gas washing pond enters solution filtering-condensing apparatus;
The CuO precipitations being filtrated to get are reclaimed by washing, can be put into gas washing pond and are continuing with;The liquid being concentrated to give is through peroxidating
Crystallization can obtain ammonium sulfate.
Some specific embodiments for preparing absorbing liquid are given below:
Embodiment 1:By gas mixing device as shown in Figure 1, flue gas simulation gas is prepared, it is 100ml/min to control gas velocity,
NO concentration is 950ppm.Weigh 0.05mol ammonium sulfite and 2.5ml ethanol deionized water dissolving and be diluted to 250ml,
Tubular type bubbling reactor is placed in, is passed through hybrid analog-digital simulation gas.As a result as shown in Figure 4, NO removal efficiency can reach 75% or so, turn
The pollution gas of change can be suppressed to less than 15%.
Embodiment 2:
The absorbefacient preparation method of particle diameter d≤20 μm:
50g copper nitrates are placed in tube furnace and prepare CuO, 600 DEG C is warming up to 5 DEG C/min heating rate and maintains
2h, described solid phase absorbefacient is obtained after cooling, the result that XRD is characterized is shown as CuO, and the product for confirming to obtain is CuO;
SEM characterization results are as shown in Fig. 2 confirm to obtain particle diameter≤20 μm of absorbefacient.The absorbefacient 0.1g for weighing to obtain is placed on
In 10ml vial, 4ml deionized waters and magneton are added, and stir 10h.
The absorbefacient preparation method of particle diameter d≤1 μm:
Buffer solution system is configured, 5.4g chloride leaches are slowly added dropwise 35ml ammoniacal liquor and be diluted in 50mL water
100mL;Weigh 0.1mol copper nitrates solid to dissolve with minimal amount of water, be slowly added dropwise into cushioning liquid, precipitated;Spend
Ion is washed three times, and ethanol is washed three times, is placed in 80 DEG C of oven for drying;Obtained solid is placed on inside tube furnace and calcined, with 5 DEG C/
Min heating rate is warming up to 600 DEG C and maintains 2h, and described solid phase absorbefacient, the result that XRD is characterized are obtained after cooling
CuO is shown as, the product for confirming to obtain is CuO;SEM characterization results as indicated at 3, confirm to obtain the μ of the particle diameter d of absorbefacient≤1
m.The absorbefacient 0.1g for weighing to obtain is placed in 10ml vial, adds 4ml deionized waters and magneton, and stir 10h.
Absorbefacient performance test:
Using the NO absorption process in example one, it is 100ml/min to control gas velocity, and NO concentration is 950ppm.Weigh
0.05mol ammonium sulfite and 2.5ml ethanol deionized water dissolving are simultaneously diluted to 230ml, are placed in tubular type bubbling reactor, lead to
Enter hybrid analog-digital simulation gas, pour into the mixture of absorbefacient and water, and washed with 16ml deionized waters.As a result as shown in Figure 4, NO
Removal efficiency can reach 75% or so, and the pollution gas of conversion can be suppressed to less than 15%.
Embodiment 3:
Surveyed using the activity in absorbefacient in the absorbefacient preparation method of particle diameter d≤20 μm in example two and example two
Method for testing.The dosage of absorbefacient is tested successively on ammonium sulfite scrubbing CO_2 and nitric oxide production influence.
According to experimental result, the removal efficiency of sulfur dioxide is up to 100%, and as shown in Figure 4, the dosage of absorbefacient is to denitration
Rate (75% or so) simultaneously has no significant effect, mainly to pollution gas (N2O suppression) makes NO be converted into dirt into positive correlation
The selectivity of metachromia gas is reduced to 10% or so.
If Fig. 5 is present invention test simultaneous SO_2 and NO removal pollution gas (N2O) selective result figure, 0.05M sulfurous acid
Ammonium (NS);1% surfactant (S);0.1gCuO(C1:Direct oxidation method, C2:The precipitation method);Lucifuge condition (dark);
As Fig. 6 be the present invention under the conditions of the co-catalyst of various dose test simultaneous SO_2 and NO removal results of property and
N2O selectivity result figures.
Claims (8)
1. a kind of flue gas treating process of liquid phase simultaneous SO_2 and NO removal, it is characterised in that this method includes:
After flue gas dedusting;
Ammonia spirit is prepared, and adds surfactant;
Flue gas after dedusting is passed through ammonia spirit, carries out pre- sweetening process, produces ammonium sulfite as absorbing liquid;
Absorbefacient is added in absorbing liquid, while carries out desulphurization denitration process;
Waste liquid carries out product recovery after out of stock to desulfurization, completes flue gas treatment.
2. the flue gas treating process of liquid phase simultaneous SO_2 and NO removal according to claim 1, it is characterised in that described ammonia
The concentration of the aqueous solution is 0.1~0.01mol/L.
3. the flue gas treating process of liquid phase simultaneous SO_2 and NO removal according to claim 1, it is characterised in that absorbing liquid is
0.1~0.01mol/L ammonium sulfite, and add 0.1%~2% surfactant of absorbing liquid volume, wherein surface-active
Agent is methanol, the one or more in ethanol and ethylene glycol.
4. the flue gas treating process of liquid phase simultaneous SO_2 and NO removal according to claim 1, it is characterised in that ammonium sulfite
The acid-base value of absorbing liquid maintains pH=7.5 ± 1.
5. the flue gas treating process of the liquid phase simultaneous SO_2 and NO removal according to claim 1-4, it is characterised in that absorbing liquid
Acid-base value control, be passed through speed by control ammoniacal liquor, be in the range of 25 DEG C~60 DEG C in temperature.
6. the flue gas treating process of liquid phase simultaneous SO_2 and NO removal according to claim 1, it is characterised in that described helps
Absorbent component is CuO, and particle size d≤10 μm, dosage is >=0.04g/L, and gas washing is put into after stirring 10h in aqueous
Pond.
7. the flue gas treating process of liquid phase simultaneous SO_2 and NO removal according to claim 1, it is characterised in that described production
Thing removal process is specially:Absorbefacient regenerating unit and collection of products device are set up after flue gas treating process, satiety
The absorbing liquid of sum by stirring, is cooled down, precipitation, is that ammonium sulfate crystallization comes out, and forms ammonium sulfate solids production by regenerative section
Product;The absorbefacient being filtrated to get can return to gas washing pond after washing and reuse.
8. the flue gas treating process of the liquid phase simultaneous SO_2 and NO removal according to claim 1-4, it is characterised in that flue gas
The speed that body is passed through is 0ml/min~500ml/min, and wherein the NO of flue gas concentration is 0ppm~1000ppm, SO2's
Concentration is 0ppm~1200ppm.
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Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN103041678A (en) * | 2012-12-21 | 2013-04-17 | 浙江天蓝环保技术股份有限公司 | Ammonia flue gas desulfuration and denitration combined process and device |
CN105032173A (en) * | 2015-04-25 | 2015-11-11 | 张少篪 | Device and process of ammonia-soda-process combined desulfurization and denitrification |
-
2017
- 2017-10-27 CN CN201711023106.3A patent/CN107744715A/en active Pending
Patent Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN103041678A (en) * | 2012-12-21 | 2013-04-17 | 浙江天蓝环保技术股份有限公司 | Ammonia flue gas desulfuration and denitration combined process and device |
CN105032173A (en) * | 2015-04-25 | 2015-11-11 | 张少篪 | Device and process of ammonia-soda-process combined desulfurization and denitrification |
Non-Patent Citations (2)
Title |
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杨继生编著: "《表面活性剂原理与应用》", 31 December 2012, 东南大学出版社 * |
杨飏编著: "《二氧化硫减排技术与烟气脱硫工程》", 31 January 2004, 北京:冶金工业出版社 * |
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