WO1987002023A1 - Reduction de substances polluantes a base d'azote et de carbone - Google Patents
Reduction de substances polluantes a base d'azote et de carbone Download PDFInfo
- Publication number
- WO1987002023A1 WO1987002023A1 PCT/US1986/002090 US8602090W WO8702023A1 WO 1987002023 A1 WO1987002023 A1 WO 1987002023A1 US 8602090 W US8602090 W US 8602090W WO 8702023 A1 WO8702023 A1 WO 8702023A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- urea
- process according
- effluent
- solution
- hexamethylenetetramine
- Prior art date
Links
Classifications
-
- 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
- B01D53/54—Nitrogen compounds
- B01D53/56—Nitrogen oxides
Definitions
- the present invention relates to improvements in the combustion of carbonaceous fuels, and more particularly to improvements in firing boilers with reduced emissions of carbon- and nitrogen-based pollutants.
- Carbonaceous fuels burn more completely, with reduced emissions of carbon monoxide and unburned hydrocarbons, at oxygen concentrations and combustion air/fuel ratios which permit optimized high flame temperatures.
- these temperatures are above 2000°F and typically from about 2200°F to 3000°F.
- thermal NO — the temperatures being so high that free radicals of nitrogen and oxygen are formed and chemically combine as nitrogen oxides (NO A).
- the flame temperature can be lowered to reduce NO A formation by the use of large excesses of air or fuel, or a hybrid of both processes known as staged combustion.
- these approaches create excessive carbon-based pollutants.
- Pacztowski discloses a more detailed, controlled two-stage catalytic system.
- the operating temperatures for the second catalytic stage where ammonia is utilized are preferably within the range of from 275°F to 900°F. This process and that of Jones et al unfortunately depend on the use of catalysts which create additional costs in terms of initial investment and servicing requirements.
- Lyon discloses a non-catalytic system for reducing nitrogen monoxide (NO) in a combustion effluent.
- Lyon discloses that ammonia and specified ammonia precursors, including ammonium carbonate also disclosed by Jones, et al , or their aqueous solutions, can be injected into the effluent, for mixing with the nitrogen monoxide at a temperature within the range of 1600°F to 2000°F.
- a reducing agent such as hydrogen gas or various hydrocarbons, can be mixed with the effluent to permit the reduction reaction to occur at temperatures as low as 1300°F, thereby assuring avoidance of high temperature oxidation of ammonia to nitrogen monoxide.
- Lyon points out that at temperatures above 2000°F, the use of ammonia was counterproductive — increasing NO rather than decreasing it.
- Williamson discloses the purification of acid gas-containing streams at low temperatures approaching ambient. Williamson discloses contacting the gas stream with an amine vapor in sufficient concentration such that its partial pressure is at least 5% of the total pressure of the gas stream. This system thus requires large amounts of the treating gas and requires equipment for separating that gas from the effluent upon completing the treatment.
- the present invention provides a process for reducing the concentration of nitrogen oxides in an oxygen-rich effluent from the combustion of a carbonaceous fuel.
- the process comprises injecting a solution comprising at least one additive compound selected from the group consisting of guanidine, guanidine carbonate, biguanide, guanylurea sulfate, melamine, dicyandiamide, calcium cyanamide, biuret, ljl'-azobisformamide, methylol urea, methylol urea-urea condensation product, dimethylol urea, methyl urea, dimethyl urea, and hexamethylene ⁇ tetramine, into said effluent.
- the temperature of the effluent at the point of injection, the concentration of the additive compound in the solution, and the size of the droplets in the dispersion, are selected to achieve reduction in nitrogen oxide levels in the effluent.
- a preferred embodiment of the invention provides for introducing an aqueous solution of hexamethylenetetramine and urea. Injection is preferably done at a plurality of spaced positions and at a uniform droplet size within the range of from about 10 to about 10,000 microns Sauter mean diameter. Variations of particle sizes within this broad range have been found effective to achieve uniform mixing of the additive compound with the effluent gas at a temperature in excess of 1300°F. For the purposes of this description, all temperatures herein are measured using an unshielded K-type thermocouple. Droplet sizes are determined with a Malvern 2200 instrument, utilizing a Franhofer diffraction, laser-based system. And, unless otherwise indicated, all parts and percentages are based on the weight of the composition at the particular point of reference.
- urea and materials such as ammonium carbonate, ammonium oxalate, ammonia, hydrazine, ammonium hydroxide, and various amines can be employed with the named additive compounds.
- Aqueous solutions are preferred according to the present invention due to their economy and can be employed with suitable effectiveness in most situations.
- the effective solutions will vary from saturated to dilute. While water will be an effective solvent for most applications, there are instances where other solvents may be advantageous in combination with water.
- the temperature of the effluent will have an influence on the concentration of the solution. At temperatures of from about 1300°F to about 2000°F, the solution will tend to operate effectively at high concentration, e.g., from 25 to 40 weight percent. On the other hand, at temperatures in excess of 2000°F, the solution will tend toward very dilute solutions. At these high temperatures, the water may comprise greater than 80%, 85% or 90% by weight of the solution, with the additive compound comprising as low as from about 0.5 to about 10% by weight of the solution.
- hexamethylene- tetr-amine is utilized to a greater extent than urea, being almost totally consumed during its interaction with NO A under proper conditions. It is further surprising that, when used in combination with urea, hexamethylenetetramine actually increases the utilization of the urea in reducing NO .A. Thus, hexamethylenetetramine is an enhancer for urea utilization in addition to being a superior NO A reducing agent in its own right.
- n.amed additive compounds are employed as NO A. reduction optimization and economics dictate.
- hexamethylene ⁇ tetramine will be present in an amount of at least about 25% based on the combined weight of it and the other active NO A reducer such as urea.
- Weight ratios of hexamethylenetetramine to urea of from about 1:3 to 3:1 are exemplary.
- the solution of additive compound will be dispersed uniformly within the effluent gas stream at a point where the effluent is at a temperature above 1300°F, and preferably above 1500°F.
- Large industrial boilers of the type employed for utility power plants and other large facilities will typically be water jacketted and have access only at limited points. In the most typical situation, the boiler interior can be accessed only in the area of the flame and at an area above the fl-ame, where the temperatures at full load are typically within the range of from about 2200°F to about 2600°F. For boilers operating efficiently with gas, the temperature at this point of access will typically fall within the range of from about 2100°F to about
- the additive compound solutions according to the present invention are preferably injected at a number of spaced points from nozzles which are effective to uniformly form and disperse droplets of the solutions within the flowing effluent stream to achieve uniform mixing.
- the size of the droplets of solution will be within the range of from about 10 to about 10,000, and preferably within the range of from about 50 to 10,000 microns Sauter mean diameter. At temperatures below 2000°F, droplet sizes of less than 150 microns are quite effective, while at higher temperatures the droplets should be larger, preferably larger than 500 microns.
- the concentration of the additive compound or compounds within the effluent gas should be sufficient to provide a reduction in nitrogen oxide levels.
- the additive compound will be employed at ' a molar ratio of nitrogen in the additive compound to the baseline nitrogen oxide level of from about 1 to 10 to 2 to 1, and will more preferably be within the range of from about 1 to 4 to 3 to 2.
- HMTA hexamethylenetetramine
- a Babcock & Wilcox 110 megawatt utility boiler was fired with residual fuel oil through ten Peabody burners to achieve 80 megawatt output.
- a series of medium-to-course droplet forming atomizers were positioned to inject treatment solutions into the effluent which was at an average temperature of about 1600°F. The following runs were made:
- HMTA hexamethy ⁇ lenetetramine
- Example 2 The boiler referred to in Example 2 was fired to 108 megawatt output. Treatment solutions were injected into the effluent at an average effluent temperature of about 2100°F. The products of combustion contained a level of NO which equated to about 10 moles per hour. The following runs were made:
- HMTA hexamethylenetetramine
- Example 1 The procedure of Example 1 is repeated for the additive compounds and combinations of them set forth in Table 4 below. The temperatures of the effluent, concentration of solutions, and feed rates are changed from Example 1 as indicated in Table 4.
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Environmental & Geological Engineering (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Treating Waste Gases (AREA)
- Processing Of Solid Wastes (AREA)
Abstract
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE1986906208 DE237568T1 (de) | 1985-10-04 | 1986-10-03 | Verminderung der stickstoff- und kohlenstoffhaltigen schadstoffe. |
Applications Claiming Priority (6)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US78482785A | 1985-10-04 | 1985-10-04 | |
US784,827 | 1985-10-04 | ||
US81153285A | 1985-12-20 | 1985-12-20 | |
US811,532 | 1985-12-20 | ||
US06/906,671 US4751065A (en) | 1985-12-20 | 1986-09-10 | Reduction of nitrogen- and carbon-based pollutants |
US906,671 | 1986-09-10 |
Publications (1)
Publication Number | Publication Date |
---|---|
WO1987002023A1 true WO1987002023A1 (fr) | 1987-04-09 |
Family
ID=27419819
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/US1986/002090 WO1987002023A1 (fr) | 1985-10-04 | 1986-10-03 | Reduction de substances polluantes a base d'azote et de carbone |
Country Status (3)
Country | Link |
---|---|
EP (1) | EP0237568A4 (fr) |
AU (1) | AU6408086A (fr) |
WO (1) | WO1987002023A1 (fr) |
Cited By (13)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO1988006487A1 (fr) * | 1987-03-06 | 1988-09-07 | Fuel Tech, Inc. | Procede de reduction des oxydes d'azote avec reduction au minimum de la production d'autres substances polluantes |
US4844878A (en) * | 1985-10-04 | 1989-07-04 | Fuel Tech, Inc. | Process for the reduction of nitrogen oxides in an effluent |
EP0342184A2 (fr) * | 1988-05-09 | 1989-11-15 | Waagner-Biro Aktiengesellschaft | Procédé d'élimination d'oxydes d'azote par des substances réductrices solides |
DE3823848A1 (de) * | 1988-07-14 | 1990-01-18 | Sueddeutsche Kalkstickstoff | Verfahren zur reduzierung von so(pfeil abwaerts)2(pfeil abwaerts)- und/oder no(pfeil abwaerts)x(pfeil abwaerts)-emissionen bei verbrennungsprozessen |
DE3907330A1 (de) * | 1989-03-04 | 1990-09-13 | Noell Gmbh | Abscheidungsprozess |
DE3929554A1 (de) * | 1989-09-06 | 1991-03-07 | Sueddeutsche Kalkstickstoff | Verfahren zur reduzierung von schadstoff-emissionen bei verbrennungsprozessen |
US5017347A (en) * | 1987-02-13 | 1991-05-21 | Fuel Tech, Inc. | Process for nitrogen oxides reduction and minimization of the production of other pollutants |
US5057293A (en) * | 1987-02-13 | 1991-10-15 | Fuel Tech, Inc. | Multi-stage process for reducing the concentration of pollutants in an effluent |
DE4031379A1 (de) * | 1990-04-27 | 1991-10-31 | Sueddeutsche Kalkstickstoff | Verfahren zur reduzierung von schadstoffemissionen bei verbrennungsprozessen |
DE4100645A1 (de) * | 1991-01-11 | 1992-07-16 | Hansjoerg Regler | Verfahren zur abscheidung von schadstoffen, insbesondere von sauren schadstoffen, aus gasen und abgasen |
GR880100134A (el) * | 1988-02-29 | 1994-03-31 | Fuel Tech Inc | Διαδικασία για την μείωση των οξειδίων αζώτου με ελαχιστοποίηση της παραγωγής άλλων ρυπαντών. |
EP0990463A2 (fr) * | 1998-09-29 | 2000-04-05 | AGS Jicin a.s. | Plaque réactive pour l'élimination d'impurétés gazeuses et procédé pour sa production |
US8048390B2 (en) | 2006-12-23 | 2011-11-01 | Alzchem Trostberg Gmbh | Method for the selective catalytic reduction of nitrogen oxides in exhaust gases of vehicles |
Families Citing this family (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4719092A (en) * | 1985-10-04 | 1988-01-12 | Fuel Tech, Inc. | Reduction of nitrogen-based pollutants through the use of urea solutions containing oxygenated hydrocarbon solvents |
Citations (14)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3599427A (en) * | 1969-09-22 | 1971-08-17 | Ford Motor Co | Exhaust gas purification |
DD110833A1 (fr) * | 1974-05-03 | 1975-01-12 | ||
CA968927A (en) * | 1974-10-04 | 1975-06-10 | Ontario Research Foundation | Treatment of no2 - containing gas streams |
JPS50110490A (fr) * | 1974-02-13 | 1975-08-30 | ||
JPS50118877A (fr) * | 1974-02-28 | 1975-09-17 | ||
US3988113A (en) * | 1973-08-17 | 1976-10-26 | Roberts Arnold L | Apparatus for treating engine exhaust gases |
DE2630202A1 (de) * | 1975-07-05 | 1977-02-03 | Babcock Hitachi Kk | Verfahren zum reduzieren von stickoxiden in verbrennungsabgasen |
JPS52109866A (en) * | 1976-03-11 | 1977-09-14 | Oki Electric Ind Co Ltd | Liquid epitaxial growing method |
JPS52112273A (en) * | 1976-03-18 | 1977-09-20 | Toshiba Corp | Scribing method of semiconductor wafer |
DE2752918A1 (de) * | 1977-11-26 | 1979-05-31 | Saarbergwerke Ag | Verfahren zum reinigen von abgasen |
US4208386A (en) * | 1976-03-03 | 1980-06-17 | Electric Power Research Institute, Inc. | Urea reduction of NOx in combustion effluents |
DE2926107A1 (de) * | 1979-06-28 | 1981-01-08 | Nukem Gmbh | Verfahren zur abscheidung von stickstoffoxiden aus gasen |
DE3014606A1 (de) * | 1980-04-16 | 1981-10-29 | UOP Kavag, Abteilung der UOP Inc. GmbH, 6467 Hasselroth | Kontinuierliches verfahren zur reinigung von industrieabgasen mit einem formaldehydgehalt |
DE3447616A1 (de) * | 1983-12-30 | 1985-07-11 | Skw Trostberg Ag, 8223 Trostberg | Mittel und verfahren zur gleichzeitigen entfernung von schwefel- und stickoxiden aus abgasen |
-
1986
- 1986-10-03 EP EP19860906208 patent/EP0237568A4/fr active Pending
- 1986-10-03 AU AU64080/86A patent/AU6408086A/en not_active Abandoned
- 1986-10-03 WO PCT/US1986/002090 patent/WO1987002023A1/fr not_active Application Discontinuation
Patent Citations (14)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3599427A (en) * | 1969-09-22 | 1971-08-17 | Ford Motor Co | Exhaust gas purification |
US3988113A (en) * | 1973-08-17 | 1976-10-26 | Roberts Arnold L | Apparatus for treating engine exhaust gases |
JPS50110490A (fr) * | 1974-02-13 | 1975-08-30 | ||
JPS50118877A (fr) * | 1974-02-28 | 1975-09-17 | ||
DD110833A1 (fr) * | 1974-05-03 | 1975-01-12 | ||
CA968927A (en) * | 1974-10-04 | 1975-06-10 | Ontario Research Foundation | Treatment of no2 - containing gas streams |
DE2630202A1 (de) * | 1975-07-05 | 1977-02-03 | Babcock Hitachi Kk | Verfahren zum reduzieren von stickoxiden in verbrennungsabgasen |
US4208386A (en) * | 1976-03-03 | 1980-06-17 | Electric Power Research Institute, Inc. | Urea reduction of NOx in combustion effluents |
JPS52109866A (en) * | 1976-03-11 | 1977-09-14 | Oki Electric Ind Co Ltd | Liquid epitaxial growing method |
JPS52112273A (en) * | 1976-03-18 | 1977-09-20 | Toshiba Corp | Scribing method of semiconductor wafer |
DE2752918A1 (de) * | 1977-11-26 | 1979-05-31 | Saarbergwerke Ag | Verfahren zum reinigen von abgasen |
DE2926107A1 (de) * | 1979-06-28 | 1981-01-08 | Nukem Gmbh | Verfahren zur abscheidung von stickstoffoxiden aus gasen |
DE3014606A1 (de) * | 1980-04-16 | 1981-10-29 | UOP Kavag, Abteilung der UOP Inc. GmbH, 6467 Hasselroth | Kontinuierliches verfahren zur reinigung von industrieabgasen mit einem formaldehydgehalt |
DE3447616A1 (de) * | 1983-12-30 | 1985-07-11 | Skw Trostberg Ag, 8223 Trostberg | Mittel und verfahren zur gleichzeitigen entfernung von schwefel- und stickoxiden aus abgasen |
Non-Patent Citations (6)
Title |
---|
CHEMICAL ABSTRACTS, vol. 103, no. 18, 4 November 1985, Columbus, Ohio, US; PETER WEBER: "Composition and Method for Simultaneous Separation of Sulfur Oxides and NitrogenOxides from flue Gases" page 293; column 1; * |
CHEMICAL ABSTRACTS, vol. 84, no. 12, 22 March 1976, Columbus, Ohio, US; abstract no. 19119M, JUERGEN GISBIER ET AL: "Detoxification of Waste Gases Containing Nitrogen Oxides" page 345; column 1; * |
CHEMICAL ABSTRACTS, vol. 84, no. 4, 26 January 1976, Columbus, Ohio, US; abstract no. 21673W, ALEXANDER LAWSON: "Treatment of Nitrogen Dioxide-Containing Gas Streams" page 303; column 2; * |
CHEMICAL ABSTRACTS, vol. 94, no. 26, 29 June 1981, Columbus, Ohio, US; abstract no. 213667A, HEINRICH QUI UMANN: "Separating Nitrogen Oxides from Gases" page 321; column 1; * |
CHEMICAL ABSTRACTS, vol. 96, no. 2, 11 January 1982, Columbus, Ohio, US; abstract no. 11125C, LUDWIG HIRCHE ET AL: "Continuous Purification of Industrial Waste Gases Containing Formaldehyde" page 297; column 1; * |
See also references of EP0237568A4 * |
Cited By (19)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4844878A (en) * | 1985-10-04 | 1989-07-04 | Fuel Tech, Inc. | Process for the reduction of nitrogen oxides in an effluent |
US5057293A (en) * | 1987-02-13 | 1991-10-15 | Fuel Tech, Inc. | Multi-stage process for reducing the concentration of pollutants in an effluent |
US5017347A (en) * | 1987-02-13 | 1991-05-21 | Fuel Tech, Inc. | Process for nitrogen oxides reduction and minimization of the production of other pollutants |
GB2225001A (en) * | 1987-03-06 | 1990-05-23 | Fuel Tech Inc | Process for nitrogen oxices reduction with minimization of the production of other pollutants |
WO1988006487A1 (fr) * | 1987-03-06 | 1988-09-07 | Fuel Tech, Inc. | Procede de reduction des oxydes d'azote avec reduction au minimum de la production d'autres substances polluantes |
GB2225001B (en) * | 1987-03-06 | 1991-09-04 | Fuel Tech Inc | Process for nitrogen oxides reduction with minimization of the production of other pollutants |
GR880100134A (el) * | 1988-02-29 | 1994-03-31 | Fuel Tech Inc | Διαδικασία για την μείωση των οξειδίων αζώτου με ελαχιστοποίηση της παραγωγής άλλων ρυπαντών. |
EP0342184A2 (fr) * | 1988-05-09 | 1989-11-15 | Waagner-Biro Aktiengesellschaft | Procédé d'élimination d'oxydes d'azote par des substances réductrices solides |
EP0342184A3 (fr) * | 1988-05-09 | 1990-03-14 | Waagner-Biro Aktiengesellschaft | Procédé d'élimination d'oxydes d'azote par des substances réductrices solides |
DE3823848A1 (de) * | 1988-07-14 | 1990-01-18 | Sueddeutsche Kalkstickstoff | Verfahren zur reduzierung von so(pfeil abwaerts)2(pfeil abwaerts)- und/oder no(pfeil abwaerts)x(pfeil abwaerts)-emissionen bei verbrennungsprozessen |
DE3907330A1 (de) * | 1989-03-04 | 1990-09-13 | Noell Gmbh | Abscheidungsprozess |
EP0416562A1 (fr) * | 1989-09-06 | 1991-03-13 | SKW Trostberg Aktiengesellschaft | Procédé pour la réduction d'émissions de polluants par procédés de combustion |
DE3929554A1 (de) * | 1989-09-06 | 1991-03-07 | Sueddeutsche Kalkstickstoff | Verfahren zur reduzierung von schadstoff-emissionen bei verbrennungsprozessen |
DE4031379A1 (de) * | 1990-04-27 | 1991-10-31 | Sueddeutsche Kalkstickstoff | Verfahren zur reduzierung von schadstoffemissionen bei verbrennungsprozessen |
DE4100645A1 (de) * | 1991-01-11 | 1992-07-16 | Hansjoerg Regler | Verfahren zur abscheidung von schadstoffen, insbesondere von sauren schadstoffen, aus gasen und abgasen |
EP0990463A2 (fr) * | 1998-09-29 | 2000-04-05 | AGS Jicin a.s. | Plaque réactive pour l'élimination d'impurétés gazeuses et procédé pour sa production |
EP0990463A3 (fr) * | 1998-09-29 | 2000-04-12 | AGS Jicin a.s. | Plaque réactive pour l'élimination d'impurétés gazeuses et procédé pour sa production |
US8048390B2 (en) | 2006-12-23 | 2011-11-01 | Alzchem Trostberg Gmbh | Method for the selective catalytic reduction of nitrogen oxides in exhaust gases of vehicles |
US8652426B2 (en) | 2006-12-23 | 2014-02-18 | Alzchem Trostberg Gmbh | Use of aqueous guanidinium formate solutions for the selective catalytic reduction of nitrogen oxides in exhaust gases of vehicles |
Also Published As
Publication number | Publication date |
---|---|
AU6408086A (en) | 1987-04-24 |
EP0237568A4 (fr) | 1989-01-24 |
EP0237568A1 (fr) | 1987-09-23 |
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