US20050002842A1 - Nox hg and so2 removal using ammonia - Google Patents
Nox hg and so2 removal using ammonia Download PDFInfo
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- US20050002842A1 US20050002842A1 US10/497,888 US49788804A US2005002842A1 US 20050002842 A1 US20050002842 A1 US 20050002842A1 US 49788804 A US49788804 A US 49788804A US 2005002842 A1 US2005002842 A1 US 2005002842A1
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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
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/60—Simultaneously removing sulfur oxides and nitrogen oxides
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/30—Alkali metal compounds
- B01D2251/304—Alkali metal compounds of sodium
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/60—Inorganic bases or salts
- B01D2251/604—Hydroxides
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
Definitions
- This invention relates to methods and apparatuses for removing NOx and SO 2 from a gas stream.
- Fossil fuels are burned in many industrial processes. Electric power producers, for example, burn large quantities of coal, oil, and natural gas. Sulfur dioxide (“SO 2 ”), nitrogen oxide (“NO”), and nitrogen dioxide (“NO 2 ”) are some of the unwanted byproducts of burning any type of fossil fuel. Mercury (“Hg”) is often also found in fossil fuels. These byproducts are known to have serious negative health effects on people, animals, and plants, and a great deal of research has been done to find a way to economically remove them from flue gas streams before they enter the atmosphere.
- SO 2 is often removed from gas streams (“desulfurization”) by scrubbing the gas with an aqueous ammonium sulfate solution containing ammonia.
- Examples of this process are disclosed in U.S. Pat. Nos. 4,690,807, 5,362,458, 6,277,343, and 6,221,325, which are not admitted to be prior art by their mention in this Background section.
- the absorbed sulfur compounds react with ammonia to form ammonium sulfite and ammonium bisulfite, which are then oxidized to form ammonium sulfate and ammonium bisulfate.
- the ammonium bisulfate is further ammoniated to form ammonium sulfate.
- the process does not remove NO or NO 2 , however, which must then be dealt with using a different process.
- NO and NO 2 can be removed from a gas stream by contacting the gas stream with either ClO 2 or O 3 to convert NO into NO 2 , and then scrubbing with an aqueous solution of a sulfur-containing reducing compound of alkali metals or ammonia, and a catalytic compound.
- a sulfur-containing reducing compound of alkali metals or ammonia and a catalytic compound.
- Ammonia aerosols are formed by gas phase reactions of ammonia vapor in the scrubber and create a blue haze or white vapor that emanates from the stack. This is also called “ammonia slip.” Free ammonia in the atmosphere would be a serious health and environmental hazard. Firnhaber dismisses the possibility of aerosol removal means due to prohibitive investment costs and high pressure loss, for instance.
- the present invention is directed to a process and apparatus that removes SO 2 , NO, and NO 2 from a gas stream that does not require the addition of a catalyst, chlorine, or ozone, occurs at a relatively high pH, and does not result in ammonia slip.
- a process that satisfies these needs comprises the steps of oxidizing NO to NO 2 , scrubbing SO 2 , NO, and NO 2 from the flue gas stream with an ammonia scrubbing solution having a pH between six and eight, and removing any ammonia aerosols generated by the scrubbing steps with an aerosol removal means.
- FIG. 1 is a process flow chart showing the process of the present invention.
- FIG. 2 is a cut-away view of an apparatus according to the present invention.
- the present invention is a process and apparatus for removing SO 2 , NO, and NO 2 from a gas stream, especially from the flue gas stream of a fossil fuel boiler.
- flue gas from the combustion of fossil fuel nearly always contains more NO than NO 2 , and often contains Hg, which can also be removed from the gas stream by this invention.
- U.S. Pat. Nos. 5,871,703, and 6,117,403 teach the use of an electrical discharge apparatus to oxidize SO 2 and NOx to form sulfuric and nitric acids respectively, collecting the acids in a wet electrostatic precipitator (“WESP”) to form an effluent, and processing the effluent to make industrial grade acids that can be sold.
- WESP wet electrostatic precipitator
- the inventors on these two patents are Alix, Neister, and McLarnon, two of whom are inventors of the present invention.
- the present invention comprises a three-step process as shown in FIG. 1 .
- a gas stream comprising SO 2 , NO, NO 2 , and perhaps Hg, are present prior to the first step 60 .
- the first step 60 is oxidizing at least a portion of the NO in the flue gas to NO 2 with an oxidizing means.
- the means selected should be able to oxidize greater than about two percent of the NO to NO 2 , and is preferably in the region of about ninety percent.
- the oxidizing step should be adjusted so that the resulting mole ratio of SO 2 to NO 2 after the oxidizing step should be at least 2.5 to 1.
- the ratio is preferably four to one, but can be greater.
- the oxidizing means 60 can be any means known in the art, including but not limited to using an electrical discharge reactor, and injecting ClO 2 , O 3 or certain organic compounds.
- U.S. Pat. Nos. 4,029,739 and 4,035,470 teach converting NO to NO 2 by the addition of ClO 2 or O 3 into the gas stream.
- U.S. Pat. No. 4,971,777 teaches the addition of certain organic compounds that decompose into radicals at high temperatures.
- Suitable electrical discharge reactors include corona, pulsed corona, e-beam, and DBD.
- DBD is synonymously referred to as silent discharge and non-thermal plasma discharge. It is not the same as corona discharge or pulsed corona discharge.
- the preferred embodiment uses a DBD reactor, such as that disclosed in U.S. Pat. No. 6,132,692, by Alix, et al.
- the operator of the process will adjust the power input to the reactor to attain the desired oxidation results as a function of the cost of power input to the reactor, desired scrubbing results, and other factors. Laboratory testing has shown that oxidation of at least 90% of the NO and Hg is readily attainable with the present invention.
- a DBD reactor will oxidize at least a portion of the NO and NO 2 in a gas stream to nitric acid, and at least a portion of the SO 2 in a gas stream to sulfuric acid. These acids are dealt with in the next step of the process.
- Hg may or may not be oxidized to HgO.
- NO and NO 2 becomes further oxidized to form HNO 3 regardless of the means used. The reason why this may be desirable will be made clear later in this specification.
- Another oxidizing means 60 is adding ethylene or propylene to the flue gas followed by oxidizing NO to NO 2 in the electrical discharge reactor. This would have the advantage of reducing the power input requirement of the electrical discharge reactor to get the same amount of NO to NO 2 oxidation.
- Ethylene can be added in about a 2:1 molar ratio of ethylene to NO.
- the chemical reaction mechanisms for ethylene conversion of NO to NO 2 in an electrical discharge reactor are likely to be as follows: C 2 H 4 +OH-->HOCH 2 CH 2 (1) HOCH 2 CH 2 +O 2 -->HOC 2 H 4 OO (2) NO+HOC 2 H 4 OO-->NO 2 +HOC 2 H 4 O (3) HOC 2 H 4 O+O 2 -->HOCH 2 CHO+HO 2 (4) NO+HO 2 -->NO 2 +OH (5)
- the output gas stream comprises less NO, more NO 2 , SO 2 , perhaps HNO 3 , perhaps H 2 SO 4 , and perhaps HgO, as shown in FIG. 1 .
- the second step 62 is scrubbing at least a portion of the SO 2 , NO, and NO 2 present in the gas stream with an aqueous ammonia scrubbing solution.
- scrubbing typically means “absorbing” to people having skill in the art, meaning that SO 2 , NO, and NO 2 is absorbed by the aqueous solution.
- scrubbing as used in this specification also includes adding anhydrous ammonia gas to initiate the reactions leading to the oxidation of SO 2 and reduction of NO 2 .
- the solution preferably comprises ammonia, ammonium sulfite, ammonium sulfate, and water.
- the solution preferably has a pH between six and eight, which is much higher than that taught by Firnhaber. Firnhaber teaches that the pH must be kept to less than five, and is preferably 4.5, to prevent the formation of aerosols.
- the present invention is not concerned with avoiding the formation of aerosols because it includes an aerosol removal means 64 , described later in this specification.
- Maintaining a relatively high pH has several benefits. It increases the speed of absorption of SO 2 . It increases the ratio of sulfite available in solution compared to bisulfite, which facilitates the oxidation of SO 2 and reduction of NO 2 . The ratio of sulfite to bisulfite is highly dependent on pH level. From these benefits, it follows that the absorption vessel, shown as item 44 in FIG. 2 , can be substantially smaller than that used to scrub the same amount of SO 2 in a conventional limestone scrubber which is the most typical SO 2 scrubber in use today. In addition, the amount of scrubbing liquid required and the liquid to gas ratio can be reduced. It is estimated that the size of the absorption vessel 44 can be reduced by half, and the liquid to gas ratio can be reduced by a third. Because the cost of the absorption vessel and liquid circulating equipment represent a large fraction of the total cost of a scrubber, the ability to substantially reduce the size of the vessel and associated pumps and piping is a major advantage of the present invention over the prior art.
- FIG. 1 shows ammonia being added at this step
- ammonia in the form of ammonium hydroxide can be added instead.
- the ammonia reacts with the gas stream output from the oxidizing step, forming ammonium sulfite and ammonium bisulfite.
- the likely chemical reactions in this step are as follows: NH 3 +H 2 O+SO 2 -->NH 4 HSO 3 (6) NH 4 HSO 3 +NH 3 -->(NH 4 ) 2 SO 3 (7) 2NH 4 OH+SO 2 -->(NH 4 ) 2 SO 3 +H 2 O (8)
- An oxidation inhibitor can be added at this step to inhibit the oxidation of sulfite to sulfate before the sulfite can perform its NO 2 reduction function.
- oxidation inhibitors include thiosulfate and thiourea.
- ammonium bisulfite and ammonium sulfite reacts with the NO and NO 2 to form ammonium sulfate.
- Ammonium sulfate is well known as a valuable agricultural fertilizer. The likely reactions that take place in this step are as follows: 2NO 2 +4(NH 4 ) 2 SO 3 -->4(NH 4 ) 2 SO 4 +N 2 (9) NO+NO 2 +3(NH 4 ) 2 SO 3 -->3(NH 4 ) 2 SO 4 +N 2 (10)
- the gas stream after the scrubbing step comprises nitrogen and water. Since the pH of the scrubbing solution is higher than about five, the output from the scrubbing step will likely contain ammonia aerosols. If not collected in the scrubbing solution, the gas stream will also contain HgO.
- the third step 64 is removing at least a portion of the ammonia aerosols and the HgO, if present, from the gas stream.
- a wet electrostatic precipitator (“WESP”) may be used as the aerosol removal means.
- WESP is effective at collecting ammonia aerosols, HgO, and any other aerosols or particles that may be present in the gas stream.
- the output of the aerosol removal means comprises N 2 as a result of the process of the present invention.
- FIG. 2 An apparatus according to the present invention is shown in FIG. 2 .
- a gas stream comprising SO 2 , NO, NO 2 , and perhaps Hg 14 enters the apparatus assisted by a forced draft fan 12 .
- the gas then enters a means for oxidizing 10 at least a portion of the NO in the gas stream to NO 2 .
- the oxidation means 10 performs the oxidizing step 60 shown in FIG. 1 , which is more fully described above.
- at least one DBD reactor is used, and can be provided in modules 16 to facilitate manufacture and installation.
- At least one power supply and controller is required to operate a DBD reactor, which are selected by those having skill in the art, but are not shown in the drawings.
- the gas stream 18 comprises SO 2 , less NO, more NO 2 , perhaps HNO 3 , perhaps H 2 SO 4 and perhaps HgO.
- the gas stream temperature at this point is about 177° C. (350° F.).
- the gas stream then enters a scrubbing vessel 44 in a region 19 over an aqueous ammonium sulfate solution 22 .
- the aqueous ammonium sulfate solution comprises ammonia, ammonium sulfite, ammonium sulfate, and water.
- the removed ammonium sulfate solution 15 can processed by industry standard means to produce a saleable fertilizer product.
- Air or other oxidizers 17 may be introduced into the ammonium sulfate solution 22 for oxidizing ammonium sulfite into ammonium sulfate.
- Ammonium sulfate solution 22 is pumped with a circulation pump 50 to a set of lower spray nozzles 24 that serve to cool and saturate the gas stream 18 with water vapor, and to a bubble cap tray 36 to absorb ammonia vapors.
- Another circulation loop is provided wherein aqueous ammonium sulfite and sulfate in a vessel 48 is pumped with a circulation pump 52 to a set of upper spray nozzles 34 . The liquid then falls to a dual flow tray 30 . A separator tray 26 allows some of the liquid to fall into the ammonium sulfate solution 22 , and the remainder is piped to the vessel 48 . Additional makeup ammonia 32 is added to the upper spray nozzles 34 .
- These two circulation loops independently or together, perform the scrubbing step 62 of FIG. 1 , which is described in detail above.
- a WESP 40 is provided to remove any ammonia aerosols or HgO that may have formed earlier in the process.
- the WESP 40 is preferably a shell-and-tube type of WESP, but can be a plate type, or any WESP such as is known by those having skill in the art.
- the WESP 40 is wetted using a set of sprays 42 fed with water via a conduit 20 .
- a mist eliminator 38 can be provided below the WESP 40 .
- the WESP 40 is an example of the aerosol removal means 64 described in FIG. 1 .
- the gas stream 46 exiting the WESP 40 has considerably less NOx and SO 2 than that which entered the process and apparatus, and has an increased amount of the reaction products, which are nitrogen and water.
- Tests were conducted in a laboratory test facility for the NO oxidizing, scrubbing, and aerosol removal steps of the process of the present invention.
- the equipment consisted of a simulated flue gas delivery system, a coaxial cylinder DBD reactor, a packed column scrubber and a tubular WESP.
- Simulated flue gas was delivered to the DBD reactor at a flow rate of 14 scfm, a temperature of 290° F.
- the three-step process and apparatus described herein was designed specifically to treat flue gas from a coal fired power plant.
- the invention is capable of operating on any gas stream in which NOx and SO 2 are present, including but not limited to gas and oil-fired boilers and various chemical manufacturing processes.
- NOx and SO 2 concentrations and operating conditions will be different in each situation. Therefore, it is understood that an operator or system designer will be motivated to modify the scrubbing step 62 to possibly eliminate the need for either one or both the oxidizing step 60 or the aerosol removal step 64 , or combine the three elements somehow so that fewer than three steps are needed.
Abstract
A process and apparatus for removing SO?2#191, NO, and NO?2#191 from a gas stream having the steps of oxidizing (60) a portion of the NO in the flue gas stream to NO?2#191, scrubbing (62) the SO?2#191, NO, and NO?2#191 with an ammonia scrubbing solution, and removing (64) any ammonia aerosols generated by the scrubbing in a wet electrostatic precipitator. The process can also remove Hg by oxidizing it to HgO and removing it in the wet electrostatic precipitator. Ammonium sulfate, a valuable fertilizer, can be withdrawn from the scrubbing solution.
Description
- a. Field of the Invention
- This invention relates to methods and apparatuses for removing NOx and SO2 from a gas stream.
- b. Description of the Related Art
- Fossil fuels are burned in many industrial processes. Electric power producers, for example, burn large quantities of coal, oil, and natural gas. Sulfur dioxide (“SO2”), nitrogen oxide (“NO”), and nitrogen dioxide (“NO2”) are some of the unwanted byproducts of burning any type of fossil fuel. Mercury (“Hg”) is often also found in fossil fuels. These byproducts are known to have serious negative health effects on people, animals, and plants, and a great deal of research has been done to find a way to economically remove them from flue gas streams before they enter the atmosphere.
- SO2 is often removed from gas streams (“desulfurization”) by scrubbing the gas with an aqueous ammonium sulfate solution containing ammonia. Examples of this process are disclosed in U.S. Pat. Nos. 4,690,807, 5,362,458, 6,277,343, and 6,221,325, which are not admitted to be prior art by their mention in this Background section. The absorbed sulfur compounds react with ammonia to form ammonium sulfite and ammonium bisulfite, which are then oxidized to form ammonium sulfate and ammonium bisulfate. The ammonium bisulfate is further ammoniated to form ammonium sulfate. The process does not remove NO or NO2, however, which must then be dealt with using a different process.
- NO and NO2 (together known as “NOx”) can be removed from a gas stream by contacting the gas stream with either ClO2 or O3 to convert NO into NO2, and then scrubbing with an aqueous solution of a sulfur-containing reducing compound of alkali metals or ammonia, and a catalytic compound. Such a process is disclosed in U.S. Pat. No. 4,029,739, by Senjo et al., which is not admitted to be prior art by its mention in this Background section. This process, however, does not remove SO2, and requires the addition of chlorine or ozone into the system by some other means.
- Some processes exist that remove both NOx and SO2. In one such process disclosed in U.S. Pat. No. 4,035,470, by Senjo et al., which is not admitted to being prior art by its mention in this Background section, NO is oxidized to NO2 by contacting the gas with either ClO2 or O3 as above. Then the SO2 is scrubbed with a sulfite and an oxidation retardant that suppresses oxidation of the sulfite to sulfate. Iron or copper compounds can also be added to depress oxidation. Optionally, ammonium hydroxide can be added to make sulfite and to react with CO2 in the gas stream to make carbonate. Like in U.S. Pat. No. 4,029,739 mentioned above, this process requires the addition of either chlorine or ozone, and further requires a consumable sulfite oxidation retardant. The referenced patent did not mention whether the byproducts included any valuable material like ammonium sulfate. However, both U.S. Pat. Nos. 4,029,739 and 4,035,470 require the addition of chlorine to a gas stream that is eventually released to the atmosphere, creating a serious safety concern.
- Yet another process for removing NOx and SO2 from a gas stream is disclosed in U.S. Pat. No. 4,971,777, by Firnhaber et al., which is not admitted to be prior art by its inclusion in this Background section. In this process, NO is oxidized to NO2 by the addition of organic compounds which decompose into radicals at high temperatures. Then an aqueous ammonia solution in which the pH is adjusted to be below 5.0 absorbs the NOx and SO2. Firnhaber teaches the importance of holding the scrubbing solution to a low pH, since higher pH levels produce aerosols of the ammonia salts that he says is an environmental burden to be thwarted. Ammonia aerosols are formed by gas phase reactions of ammonia vapor in the scrubber and create a blue haze or white vapor that emanates from the stack. This is also called “ammonia slip.” Free ammonia in the atmosphere would be a serious health and environmental hazard. Firnhaber dismisses the possibility of aerosol removal means due to prohibitive investment costs and high pressure loss, for instance.
- What is needed, therefore, is a cost-effective process that removes SO2, NO, and NO2 from a gas stream that does not require the addition of a catalyst, chlorine, or ozone, can occur at relatively high pH, and does not result in ammonia slip.
- The present invention is directed to a process and apparatus that removes SO2, NO, and NO2 from a gas stream that does not require the addition of a catalyst, chlorine, or ozone, occurs at a relatively high pH, and does not result in ammonia slip. A process that satisfies these needs comprises the steps of oxidizing NO to NO2, scrubbing SO2, NO, and NO2 from the flue gas stream with an ammonia scrubbing solution having a pH between six and eight, and removing any ammonia aerosols generated by the scrubbing steps with an aerosol removal means. These and other features, aspects, and advantages of the present invention will become better understood with reference to the following description, drawings, and claims.
-
FIG. 1 is a process flow chart showing the process of the present invention. -
FIG. 2 is a cut-away view of an apparatus according to the present invention. - The present invention is a process and apparatus for removing SO2, NO, and NO2 from a gas stream, especially from the flue gas stream of a fossil fuel boiler. In practice, flue gas from the combustion of fossil fuel nearly always contains more NO than NO2, and often contains Hg, which can also be removed from the gas stream by this invention.
- The inventors are familiar with methods and apparatuses for removing SO2 and NOx from gas streams. U.S. Pat. Nos. 5,871,703, and 6,117,403 teach the use of an electrical discharge apparatus to oxidize SO2 and NOx to form sulfuric and nitric acids respectively, collecting the acids in a wet electrostatic precipitator (“WESP”) to form an effluent, and processing the effluent to make industrial grade acids that can be sold. The inventors on these two patents are Alix, Neister, and McLarnon, two of whom are inventors of the present invention. U.S. Pat. No. 6,132,692 teaches the use of a dielectric barrier discharge (“DBD”) reactor to form the same acids, collecting them in a WESP, and draining them from the WESP to remove them from a gas stream. The inventors on this patent are Alix, Neister, McLarnon, and Boyle, two of whom are inventors of the present invention. The above three patents were owned by the owner of the present invention as of the filing date of this specification. They are hereby incorporated by reference as if completely rewritten herein.
- The present invention comprises a three-step process as shown in
FIG. 1 . A gas stream comprising SO2, NO, NO2, and perhaps Hg, are present prior to thefirst step 60. Thefirst step 60 is oxidizing at least a portion of the NO in the flue gas to NO2 with an oxidizing means. The means selected should be able to oxidize greater than about two percent of the NO to NO2, and is preferably in the region of about ninety percent. - The oxidizing step should be adjusted so that the resulting mole ratio of SO2 to NO2 after the oxidizing step should be at least 2.5 to 1. The ratio is preferably four to one, but can be greater. The oxidizing means 60 can be any means known in the art, including but not limited to using an electrical discharge reactor, and injecting ClO2, O3 or certain organic compounds. For example, U.S. Pat. Nos. 4,029,739 and 4,035,470 teach converting NO to NO2 by the addition of ClO2 or O3 into the gas stream. U.S. Pat. No. 4,971,777 teaches the addition of certain organic compounds that decompose into radicals at high temperatures.
- Examples of suitable electrical discharge reactors include corona, pulsed corona, e-beam, and DBD. DBD is synonymously referred to as silent discharge and non-thermal plasma discharge. It is not the same as corona discharge or pulsed corona discharge. The preferred embodiment uses a DBD reactor, such as that disclosed in U.S. Pat. No. 6,132,692, by Alix, et al. In practice, the operator of the process will adjust the power input to the reactor to attain the desired oxidation results as a function of the cost of power input to the reactor, desired scrubbing results, and other factors. Laboratory testing has shown that oxidation of at least 90% of the NO and Hg is readily attainable with the present invention.
- As taught in U.S. Pat. No. 6,132,692, a DBD reactor will oxidize at least a portion of the NO and NO2 in a gas stream to nitric acid, and at least a portion of the SO2 in a gas stream to sulfuric acid. These acids are dealt with in the next step of the process.
- If oxidizing means other than an electrical discharge reactor is used, Hg may or may not be oxidized to HgO. On the other hand, it is possible, and perhaps desirable, that some of the NO and NO2 becomes further oxidized to form HNO3 regardless of the means used. The reason why this may be desirable will be made clear later in this specification.
- Another oxidizing means 60 is adding ethylene or propylene to the flue gas followed by oxidizing NO to NO2 in the electrical discharge reactor. This would have the advantage of reducing the power input requirement of the electrical discharge reactor to get the same amount of NO to NO2 oxidation. Ethylene can be added in about a 2:1 molar ratio of ethylene to NO. The chemical reaction mechanisms for ethylene conversion of NO to NO2 in an electrical discharge reactor are likely to be as follows:
C2H4+OH-->HOCH2CH2 (1)
HOCH2CH2+O2-->HOC2H4OO (2)
NO+HOC2H4OO-->NO2+HOC2H4O (3)
HOC2H4O+O2-->HOCH2CHO+HO2 (4)
NO+HO2-->NO2+OH (5)
In any event, the output gas stream comprises less NO, more NO2, SO2, perhaps HNO3, perhaps H2SO4, and perhaps HgO, as shown inFIG. 1 . - The
second step 62 is scrubbing at least a portion of the SO2, NO, and NO2 present in the gas stream with an aqueous ammonia scrubbing solution. The term “scrubbing” typically means “absorbing” to people having skill in the art, meaning that SO2, NO, and NO2 is absorbed by the aqueous solution. However, it is intended that the term “scrubbing”as used in this specification also includes adding anhydrous ammonia gas to initiate the reactions leading to the oxidation of SO2 and reduction of NO2. - The solution preferably comprises ammonia, ammonium sulfite, ammonium sulfate, and water. The solution preferably has a pH between six and eight, which is much higher than that taught by Firnhaber. Firnhaber teaches that the pH must be kept to less than five, and is preferably 4.5, to prevent the formation of aerosols. However, the present invention is not concerned with avoiding the formation of aerosols because it includes an aerosol removal means 64, described later in this specification.
- Maintaining a relatively high pH has several benefits. It increases the speed of absorption of SO2. It increases the ratio of sulfite available in solution compared to bisulfite, which facilitates the oxidation of SO2 and reduction of NO2. The ratio of sulfite to bisulfite is highly dependent on pH level. From these benefits, it follows that the absorption vessel, shown as
item 44 inFIG. 2 , can be substantially smaller than that used to scrub the same amount of SO2 in a conventional limestone scrubber which is the most typical SO2 scrubber in use today. In addition, the amount of scrubbing liquid required and the liquid to gas ratio can be reduced. It is estimated that the size of theabsorption vessel 44 can be reduced by half, and the liquid to gas ratio can be reduced by a third. Because the cost of the absorption vessel and liquid circulating equipment represent a large fraction of the total cost of a scrubber, the ability to substantially reduce the size of the vessel and associated pumps and piping is a major advantage of the present invention over the prior art. - Although
FIG. 1 shows ammonia being added at this step, ammonia in the form of ammonium hydroxide can be added instead. The ammonia reacts with the gas stream output from the oxidizing step, forming ammonium sulfite and ammonium bisulfite. The likely chemical reactions in this step are as follows:
NH3+H2O+SO2-->NH4HSO3 (6)
NH4HSO3+NH3-->(NH4)2SO3 (7)
2NH4OH+SO2-->(NH4)2SO3+H2O (8) - An oxidation inhibitor can be added at this step to inhibit the oxidation of sulfite to sulfate before the sulfite can perform its NO2 reduction function. Examples of oxidation inhibitors include thiosulfate and thiourea.
- The ammonium bisulfite and ammonium sulfite reacts with the NO and NO2 to form ammonium sulfate. Ammonium sulfate is well known as a valuable agricultural fertilizer. The likely reactions that take place in this step are as follows:
2NO2+4(NH4)2SO3-->4(NH4)2SO4+N2 (9)
NO+NO2+3(NH4)2SO3-->3(NH4)2SO4+N2 (10) - Most of the HNO3 that may have been formed by further oxidation of NO and NO2, and/or created by a DBD reactor, will react with ammonia and form ammonium nitrate, also known to be a valuable agricultural fertilizer, according to the following formula:
HNO3+NH3-->NH4NO3 (11) - In a similar way, most of the sulfuric acid created by the DBD reactor will react with the solution and form ammonium bisulfate and ammonium sulfate. As one can see from the above equations, the process removes SO2, NO, and NO2 from the gas stream, and produces ammonium nitrate, ammonium sulfate, and nitrogen. Over time, the ammonium sulfate and ammonium nitrate will concentrate in the aqueous ammonia solution and precipitate out of solution. The solid precipitate can then be removed from the scrubber and processed for use as fertilizer.
- The gas stream after the scrubbing step comprises nitrogen and water. Since the pH of the scrubbing solution is higher than about five, the output from the scrubbing step will likely contain ammonia aerosols. If not collected in the scrubbing solution, the gas stream will also contain HgO.
- The
third step 64 is removing at least a portion of the ammonia aerosols and the HgO, if present, from the gas stream. A wet electrostatic precipitator (“WESP”) may be used as the aerosol removal means. A WESP is effective at collecting ammonia aerosols, HgO, and any other aerosols or particles that may be present in the gas stream. - As a result of this three-step process, SO2, NO, NO2, and Hg are removed from a gas stream to provide ammonium sulfate and ammonium nitrate. The output of the aerosol removal means comprises N2 as a result of the process of the present invention.
- An apparatus according to the present invention is shown in
FIG. 2 . A gas stream comprising SO2, NO, NO2, and perhapsHg 14 enters the apparatus assisted by a forceddraft fan 12. The gas then enters a means for oxidizing 10 at least a portion of the NO in the gas stream to NO2. The oxidation means 10 performs the oxidizingstep 60 shown inFIG. 1 , which is more fully described above. In the preferred embodiment, at least one DBD reactor is used, and can be provided inmodules 16 to facilitate manufacture and installation. At least one power supply and controller is required to operate a DBD reactor, which are selected by those having skill in the art, but are not shown in the drawings. - After the oxidation means 10, the
gas stream 18 comprises SO2, less NO, more NO2, perhaps HNO3, perhaps H2SO4 and perhaps HgO. The gas stream temperature at this point is about 177° C. (350° F.). The gas stream then enters a scrubbingvessel 44 in aregion 19 over an aqueousammonium sulfate solution 22. Preferably, the aqueous ammonium sulfate solution comprises ammonia, ammonium sulfite, ammonium sulfate, and water. Water in theammonium sulfate solution 22 evaporates due to the heat of thegas stream 18, thus concentrating ammonium sulfate solution 15, which is then removed from thevessel 44. The removed ammonium sulfate solution 15 can processed by industry standard means to produce a saleable fertilizer product. - Air or
other oxidizers 17 may be introduced into theammonium sulfate solution 22 for oxidizing ammonium sulfite into ammonium sulfate.Ammonium sulfate solution 22 is pumped with acirculation pump 50 to a set oflower spray nozzles 24 that serve to cool and saturate thegas stream 18 with water vapor, and to abubble cap tray 36 to absorb ammonia vapors. - Another circulation loop is provided wherein aqueous ammonium sulfite and sulfate in a
vessel 48 is pumped with acirculation pump 52 to a set ofupper spray nozzles 34. The liquid then falls to adual flow tray 30. Aseparator tray 26 allows some of the liquid to fall into theammonium sulfate solution 22, and the remainder is piped to thevessel 48.Additional makeup ammonia 32 is added to theupper spray nozzles 34. These two circulation loops, independently or together, perform the scrubbingstep 62 ofFIG. 1 , which is described in detail above. - Following the scrubbing loops, a
WESP 40 is provided to remove any ammonia aerosols or HgO that may have formed earlier in the process. TheWESP 40 is preferably a shell-and-tube type of WESP, but can be a plate type, or any WESP such as is known by those having skill in the art. TheWESP 40 is wetted using a set ofsprays 42 fed with water via aconduit 20. Amist eliminator 38 can be provided below theWESP 40. TheWESP 40 is an example of the aerosol removal means 64 described inFIG. 1 . Thegas stream 46 exiting theWESP 40 has considerably less NOx and SO2 than that which entered the process and apparatus, and has an increased amount of the reaction products, which are nitrogen and water. - The following laboratory-scale examples of the process demonstrate the efficacy of the present invention:
- An absorption test was done for the scrubbing step of the process of the present invention, with a solution that was 1% w/w SO3 2− (“sulfite”), 6% w/w SO4 2− (“sulfate”), and 2.5% S2O3 2− (“thiosulfate”) in a packed column that was 46 cm (18 inches) high and 3.8 cm (1.5 inches) in diameter. The column was packed with 0.64 cm ({fraction (1/4)} inch) glass RASCHIG rings. The simulated flue gas at the inlet of the column contained 13% v/v moisture, 6% v/v O2 and the simulated flue gas pollutants listed in the table. There was continuous addition of NH3 and (NH4)2S2O3 to maintain a pH of 6.8 and a thiosulfate concentration of 2.5% w/w. The residence time in the column was 1.8 sec with an L/G ratio of 56 lpm/kacm·hr (25 gpm/kacfm).
- The table shows the concentrations of NO, NO2, and SO2 at the inlet and outlet of the test system.
TABLE 1 Scrubbing Step Alone System Inlet System Outlet NO (ppmv) 20 4 NO2 (ppmv) 250 36 SO2 (ppmv) 1370 2 - An absorption test was done for the scrubbing step of the process of the present invention starting with water and a flue gas stream consisting of 13% v/v moisture, 17 ppmv NO, 267 ppmv NO2, 1360 ppmv SO2, 6% v/v ° 2 and balance N2. Ammonia and ammonium thiosulfate were added to maintain a pH of 6.8 and a thiosulfate concentration of 2.5%, and the concentrations of sulfite and sulfate in the system were allowed to build to steady state. The NOx removal rate was 80% w/w at concentrations of SO3 2−, SO4 2− and S2O3 2− of 0.7% w/w, 2.5% w/w, and 0.5% w/w respectively.
- Tests were conducted in a laboratory test facility for the NO oxidizing, scrubbing, and aerosol removal steps of the process of the present invention. The equipment consisted of a simulated flue gas delivery system, a coaxial cylinder DBD reactor, a packed column scrubber and a tubular WESP. The following is an example of data obtained in the lab test facility. Simulated flue gas was delivered to the DBD reactor at a flow rate of 14 scfm, a temperature of 290° F. and with the following composition: 6.2% v/v O2, 14.2% v/v CO2, 8.2% v/v H2O, 20 ppmv CO, 250 ppmv C2H4, 1740 ppmv SO2, and 259 ppmv NOx. Gas velocity through the discharge reactor was 15 m/s (50 ft/sec) with discharge power level of 140 watts. Gas from the discharge reactor entered a 10 cm (4 inch) ID packed column scrubber, packed with 1.3 cm ({fraction (1/2)} inch) INTALOX saddles to a depth of 1.2 m (4 feet). Liquid was introduced at the top of the scrubber at a flow rate of 1.2 lpm (0.33 gpm), L/G=44 lpm/kacm·hr (20 gpm/kacfm). Aqueous ammonia was added to and effluent liquid removed from the recirculating scrubber solution to maintain a constant total liquid volume and solution pH at 6.6. Gas from the packed bed scrubber was treated in a 10 cm (4 inch) ID wetted wall electrostatic precipitator with a gas residence time of 0.7 seconds. The table below shows the concentrations of NO, NO2 and SO2 at the inlet to the system, the outlet of the barrier discharge reactor and at the outlet of the system.
TABLE 2 Three Step Process Discharge Reactor System System Inlet Outlet Outlet NO (ppmv) 254 45 32 NO2 (ppmv) 5 109 9 SO2 (ppmv) 1740 1598 1 - The three-step process and apparatus described herein was designed specifically to treat flue gas from a coal fired power plant. However, it can be appreciated that the invention is capable of operating on any gas stream in which NOx and SO2 are present, including but not limited to gas and oil-fired boilers and various chemical manufacturing processes. The NOx and SO2 concentrations and operating conditions will be different in each situation. Therefore, it is understood that an operator or system designer will be motivated to modify the scrubbing
step 62 to possibly eliminate the need for either one or both the oxidizingstep 60 or theaerosol removal step 64, or combine the three elements somehow so that fewer than three steps are needed. - It will be apparent to those skilled in the art that various changes and modifications can be made without departing from the spirit of the present invention. Accordingly, it is intended to encompass within the appended claims all such changes and modifications that fall within the scope of the present invention.
Claims (29)
1. A process for removing SO2, NO, and NO2 from a gas stream comprising the steps of
a. oxidizing at least a portion of NO in a gas stream to NO2 with an oxidizing means resulting in a mole ratio of SO2 to NO2 of between 2.5 to 1 and 4 to 1, followed by
b. scrubbing at least a portion of SO2, NO, and NO2 from the gas stream with a scrubbing solution
comprising ammonia, and
having a pH between 6 and 8, and
c. removing at least a portion of any ammonia aerosols generated from the scrubbing step from the gas stream with an aerosol removal means.
2. The process of claim 1 , wherein said oxidizing means is an electrical discharge reactor.
3. The process of claim 2 , wherein said electrical discharge reactor is a dielectric barrier discharge reactor.
4. The process of claim 3 , further comprising the step of oxidizing at least a portion of the NO to HNO3 with said dielectric barrier discharge reactor.
5. The process of claim 1 , wherein said oxidizing means comprises injecting ethylene or propylene.
6. The process of claim 1 , wherein said oxidizing step is adapted to result in a mole ratio of SO2 to NO2 of at least four to one.
7. The process of claim 1 , said scrubbing solution
comprising ammonia, ammonium sulfite, ammonium sulfate, and water, and
having a pH between 6 and 8.
8. The process of claim 1 , wherein said aerosol removal means is a wet electrostatic precipitator.
9. The process of claim 1 , wherein said scrubbing step results in the formation of ammonium sulfate, the process further comprising the step of withdrawing ammonium sulfate from the scrubbing solution.
10. The process of claim 4 , wherein said scrubbing step results in the formation of ammonium nitrate, the process further comprising the step of withdrawing ammonium nitrate from the scrubbing solution.
11. A process for removing SO2, NO, NO2, and Hg from a gas stream comprising the steps of
a. oxidizing at least a portion of the NO in a gas stream to NO2, and at least a portion of the Hg in a gas stream to HgO, with an oxidizing means resulting in a mole ratio of SO2 to NO2 of between 2.5 to 1 and 4 to 1, followed by
b. scrubbing at least a portion of the SO2, NO, and NO2 from the gas stream with a scrubbing solution
comprising ammonia, and
having a pH between 6 and 8, and
c. removing at least a portion of any ammonia aerosols generated from the scrubbing step, and HgO, from the gas stream with an aerosol removal means.
12. The process of claim 11 , wherein said oxidizing means comprising a dielectric discharge reactor.
13. The process of claim 11 , wherein said oxidizing means comprising injecting ethylene or propylene.
14. The process of claim 11 , wherein said aerosol removal means is a wet electrostatic precipitator.
15. The process of claim 11 , said scrubbing solution comprising ammonia, ammonium sulfite, ammonium sulfate, and water, and having a pH between 6 and 8.
16. The process of claim 15 , wherein said scrubbing step results in the formation of ammonium sulfate, the process further comprising the step of withdrawing ammonium sulfate from the scrubbing solution.
17. An apparatus for removing SO2, NO, and NO2 from a gas stream comprising
a. an oxidizing means for oxidizing at least a portion of the NO in a gas stream to NO2, followed by
b. a scrubber suitably adapted to scrub at least a portion of the SO2, NO, and NO2 from the gas stream with a scrubbing solution
comprising ammonia, and
having a pH between 6 and 8, and
c. an aerosol removal means for removing at least a portion of any ammonia aerosols generated by the scrubber from the gas stream.
18. The apparatus of claim 17 , wherein said oxidizing means is at least one electrical discharge reactor.
19. The apparatus of claim 18 , wherein said electrical discharge reactor is at least one dielectric barrier discharge reactor.
20. The apparatus of claim 19 , wherein said dielectric barrier discharge reactor is adapted to oxidize at least a portion of the NO to NO2 and HNO3.
21. The apparatus of claim 17 , said scrubbing solution
comprising ammonia, ammonium sulfite, ammonium sulfate, and water, and having a pH between 6 and 8.
22. The apparatus of claim 17 , wherein said aerosol removal means is at least one wet electrostatic precipitator.
23. An apparatus for removing SO2, NO, NO2, and Hg from a gas stream comprising
a. an oxidizing means for oxidizing at least a portion of the NO in a gas stream to NO2, and at least a portion of the Hg in a gas stream to HgO, followed by
b. a scrubber suitably adapted to scrub at least a portion of the SO2, NO, and NO2 from the gas stream with a scrubbing solution
comprising ammonia, and
having a pH between 6 and 8, and
c. an aerosol removal means for removing at least a portion of any ammonia aerosols generated by the scrubber, and HgO, from the gas stream.
24. An apparatus for removing SO2, NO, and NO2 from a gas stream comprising
a. an NO oxidizer adapted to oxidize at least a portion of the NO in a gas stream to NO2, followed by
b. a scrubber adapted to scrub at least a portion of the SO2, NO, and NO2 from the gas stream with a scrubbing solution
comprising ammonia, and
having a pH between 6 and 8, and
c. an aerosol remover adapted to remove at least a portion of any ammonia aerosols generated by the scrubber from the gas stream.
25. The apparatus of claim 24 , wherein said NO oxidizer is at least one electrical discharge reactor.
26. The apparatus of claim 25 , wherein said electrical discharge reactor is at least one dielectric barrier discharge reactor.
27. The apparatus of claim 26 , wherein said dielectric barrier discharge reactor is adapted to oxidize at least a portion of the NO to NO2 and HNO3.
28. The apparatus of claim 24 , said scrubbing solution comprising ammonia, ammonium sulfite, ammonium sulfate, and water, and having a pH between 6 and 8.
29. The apparatus of claim 24 , wherein said aerosol remover is at least one wet electrostatic precipitator.
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US10/497,888 US20050002842A1 (en) | 2001-12-06 | 2002-12-06 | Nox hg and so2 removal using ammonia |
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US10/497,888 US20050002842A1 (en) | 2001-12-06 | 2002-12-06 | Nox hg and so2 removal using ammonia |
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US09/683,663 Expired - Fee Related US6605263B2 (en) | 2001-12-06 | 2002-01-31 | Sulfur dioxide removal using ammonia |
US10/064,280 Expired - Fee Related US7052662B2 (en) | 2001-12-06 | 2002-06-28 | NOx, Hg, and SO2 removal using alkali hydroxide |
US10/064,736 Expired - Fee Related US7048899B2 (en) | 2001-12-06 | 2002-08-12 | Removing NOx, SO2, and Hg from a gas stream using limestone regeneration |
US10/497,888 Abandoned US20050002842A1 (en) | 2001-12-06 | 2002-12-06 | Nox hg and so2 removal using ammonia |
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US10/064,280 Expired - Fee Related US7052662B2 (en) | 2001-12-06 | 2002-06-28 | NOx, Hg, and SO2 removal using alkali hydroxide |
US10/064,736 Expired - Fee Related US7048899B2 (en) | 2001-12-06 | 2002-08-12 | Removing NOx, SO2, and Hg from a gas stream using limestone regeneration |
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CN (1) | CN1326767C (en) |
AU (1) | AU2002359633A1 (en) |
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US20030161774A1 (en) * | 2001-07-11 | 2003-08-28 | Battelle Memorial Institute | Processes and apparatuses for treating halogen-containing gases |
US20040131524A1 (en) * | 2001-07-11 | 2004-07-08 | Battelle Memorial Institute | Processes and apparatuses for treating halogen-containing gases |
US6962679B2 (en) * | 2001-07-11 | 2005-11-08 | Battelle Memorial Institute | Processes and apparatuses for treating halogen-containing gases |
US7220396B2 (en) | 2001-07-11 | 2007-05-22 | Battelle Memorial Institute | Processes for treating halogen-containing gases |
US7407635B2 (en) | 2001-07-11 | 2008-08-05 | Battelle Memorial Institute | Processes and apparatuses for treating halogen-containing gases |
CN102160961A (en) * | 2011-02-25 | 2011-08-24 | 华北电力大学 | Dielectric barrier discharge reactor, fume desulfurization and denitration system and desulfurizating and denitrating process |
Also Published As
Publication number | Publication date |
---|---|
US20030108472A1 (en) | 2003-06-12 |
CN1326767C (en) | 2007-07-18 |
US20030108466A1 (en) | 2003-06-12 |
US20030175190A1 (en) | 2003-09-18 |
CA2469321C (en) | 2009-08-18 |
US7052662B2 (en) | 2006-05-30 |
US20030108469A1 (en) | 2003-06-12 |
US6605263B2 (en) | 2003-08-12 |
US6936231B2 (en) | 2005-08-30 |
WO2003050039A1 (en) | 2003-06-19 |
US7048899B2 (en) | 2006-05-23 |
CA2469321A1 (en) | 2003-06-19 |
HK1078303A1 (en) | 2006-03-10 |
AU2002359633A1 (en) | 2003-06-23 |
CN1617831A (en) | 2005-05-18 |
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