WO2004076035A1 - Procede de realisation de desulfuration et de denitrification - Google Patents
Procede de realisation de desulfuration et de denitrification Download PDFInfo
- Publication number
- WO2004076035A1 WO2004076035A1 PCT/JP2003/015610 JP0315610W WO2004076035A1 WO 2004076035 A1 WO2004076035 A1 WO 2004076035A1 JP 0315610 W JP0315610 W JP 0315610W WO 2004076035 A1 WO2004076035 A1 WO 2004076035A1
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- WIPO (PCT)
- Prior art keywords
- reaction
- combustion gas
- desulfurization
- combustion
- concentration
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Classifications
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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
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23J—REMOVAL OR TREATMENT OF COMBUSTION PRODUCTS OR COMBUSTION RESIDUES; FLUES
- F23J2219/00—Treatment devices
- F23J2219/20—Non-catalytic reduction devices
Definitions
- the present invention relates to a desulfurization and denitration method.
- Fossil fuels such as northern coal and heavy oil typically contain S (sulfur) as an impurity.
- S sulfur
- S_ ⁇ 2 When burning these fuels in excess air under, S is almost oxidation completely diacids I ⁇ Yellow (S_ ⁇ 2), is discharged into the atmosphere. Discharged S 0 2 becomes a major cause of acid rain, connexion not preferable environmentally because it causes deforestation and desertification associated therewith.
- various methods have been implemented conventionally, also it has been proposed. To give a few examples, the traditional method is to use a scrubber.
- v 2 0 5 by using a catalyst such as there is a method of removing S 0 2, S 0 2 to about 7 0 0 K easily it is known that can be oxidized to S 0 3 in the combustion gas temperature region (See G. Xu and 6 others, J. Chero. Engineering of Japan, 1999, Vol. 32, p. 82). Alternatively, hoping to obtain an effective by-products such as H 2 S 0 4, it is considered to be converted by Sani spoon the S 0 2 to S_ ⁇ 3.
- H 0 2 and H 2 0 2 (large under and three other people, "the development of the dry desulfurization and denitration method using a chain reaction by H_ ⁇ 2", Society of Chemical Engineers, Japan National Convention, 2 (See S108, March 30, 2002) or oxidation studies with methyl peroxyradical (CS Kan et al., 3 int. J. Chem. Kinet. , 1979, Vol. 11, p. 921), but the reaction rate constant is considered to be small under normal combustion gas conditions.
- the S_ ⁇ 2 S_ ⁇ 3 also a method for converting NO to N_ ⁇ 2, but the realization of a dry desulfurization and denitrification method is desired which does not require large amounts of water or expensive catalysts, for example, the oxidation of a stable molecule S0 2 reaction requires a high activation energy, in a typical fuel gas state, within a reasonable reaction time of less than one second is difficult.
- desulfurization and denitration method for a catalyst without thereby efficiently reacting S0 2 and NO is oxidized is not known. Disclosure of the invention
- Te desulfurization and denitrification method odor performing denitration of S 0 2 of the desulfurization and NO in the combustion gas produced from the combustion process, S_ ⁇ in the combustion gas
- a ⁇ ⁇ H radical is added to form a chain reaction to oxidize SO 2 and NO.
- a gas M that does not contribute to the reaction may be added to the combustion gas of the combustion process.
- the combustion process can be performed at atmospheric pressure. Also, this combustion process can be performed at temperatures between 650 K and 800 K.
- desulfurization treatment and denitration treatment can be performed only by adding OH radicals to the combustion gas, and the reaction can be carried out at atmospheric pressure, which is extremely simple and low cost. It is.
- Figure 1 is a constant HN0 3, a diagram showing the temperature dependence of the calculation result of the S0 3 generation concentration on NO amount.
- Figure 2 is a table showing the rate constants of the added elementary reactions.
- FIG. 3 is a view showing a calculated value of a mole fraction of sulfur compound from 400 K to 100 °.
- FIG. 6 is a diagram showing the main elementary reaction sensitivity coefficient calculation result of relative S0 3 concentration.
- Figure 8 is a view to view the temperature dependence of the calculation result of S0 3 generation concentration on HN0 3 addition amount.
- Figure 9 is reduced to the process of combustion gases containing N_ ⁇ gas S_ ⁇ 2 by HN0 3 addition It is a figure showing composition of a pressure processing device.
- Figure 10 is a diagram showing the time of processing the combustion gas using a vacuum processing apparatus shown in FIG. 9, the HN0 3 addition amount dependency of S0 3 generation amount at 750 K.
- SO 2 and N ⁇ in the combustion gas are in the left equation of the chemical reaction equation (R1) and the left equation of the chemical reaction equation (R 3).
- 0 2 is the oxygen gas contained in the combustion gases.
- M is a gas that does not contribute to the reaction, for example, N 2 , C ⁇ 2 or H 2 added simultaneously with 2 .
- H_ ⁇ _S0 2 generated reacts with ⁇ 2 in the combustion gas H_ ⁇ 2 and S_ ⁇ 3 occurs (see the chemical reaction formula (R2)).
- ⁇ 2 concentration in the fuel gas due much higher than any radical species, as reaction rate, OH + HO S_ ⁇ 2, O + HOSO2 or H + H_ ⁇ _S0 2 (R2), fast advances ⁇ than the other H OS0 2 reaction by radical species.
- Figure 1 is a constant HN0 3, a diagram showing the temperature dependence of the calculation result of the S0 3 generation concentration on NO amount.
- the horizontal axis is the temperature (K)
- the vertical axis represents S0 3 concentration (p pm).
- the calculation conditions are based on the assumption that the reaction is adiabatic, and the reaction time is 1 second.
- S_ ⁇ 2 concentration in the combustion gas is 2000 111 Deari
- ⁇ 1 ⁇ 0 3 concentration is 1 O Oppm.
- M consists N 2 and C0 2 and H 2 ⁇ , pressure when combined 0 2 in the combustion gases, as can be ignored because S0 2 concentration and HN_ ⁇ 3 concentration is very small, 1 atm (1 a tm) and the percentage (%) is'
- the simulator one Deployment is, the chemical reaction formula (R1) ⁇ (R4) calculated by the reaction mechanism of the SO x proposed by Mu e 1 1 er et al., In addition, some containing HN_ ⁇ 3 and NO 3 (See MA Mueller, RA Yetter, and F, L. Dryer, Int. J. Chem. Kinet., 32, 317 (2000)).
- Figure 2 is a table showing the rate constants of the added elementary reactions.
- the elementary reaction added is, for example, the following chemical reaction formula that inhibits the chemical reaction formula (F).
- FIG. 3 is a diagram showing the calculated values of the mole fraction of sulfur compounds from 400 K to 10000 ⁇ .
- the vertical axis is the mole fraction of the sulfur compound
- the horizontal axis is the temperature ( ⁇ ).
- S_ ⁇ 3 in 600 K ⁇ 85 OK, and are H 2 S_ ⁇ 4 and S_ ⁇ 2 O remote stable, that in particular 6 50 K ⁇ 80 OK mole fraction is the largest value Understand.
- 6 50 K ⁇ 80 OK it likely to be susceptible S_ ⁇ 2 is oxidized.
- FIG. 4 is a diagram showing a calculation result of the dependence of S ⁇ 3 generation on the NO addition concentration at T-750K.
- the vertical axis represents S0 3 concentration
- the horizontal axis represents the NO concentration (P pm). Except that HN0 3 concentration is 100 p pm are the same as the conditions in FIG. It can be seen that the conversion increases with NO concentration up to about 20 O ppm and decreases with higher NO concentration.
- Figure 6 is a diagram showing a calculation result of various chemical species of a temporal change in the oxidation reaction of S0 2 and NO in FIG.
- the vertical axis is mole fraction
- the horizontal axis is time (seconds).
- the temperature is 750 K
- conditions other than S0 2 concentration is 1 000 p pm is the same as FIG.
- oxidation N_ ⁇ and S_ ⁇ 2 by the thermal decomposition of HN_ ⁇ 3, S0 3 and N0 2 is generated not seen Rukoto about 0.2 seconds.
- the major oxidation product S0 3 and N_ ⁇ 2 NO is hardly generated, ⁇ Ka ⁇ the NO may cull to have been substantially completely oxidized to NO 2 min.
- FIG. 7 is a diagram showing calculation results of sensitivity coefficients of main elementary reactions with respect to S 0 concentration under the calculation conditions of FIG.
- the initial state is the same as in FIG.
- the vertical axis represents sensitivity coefficient of the main reaction of S_ ⁇ 3 generation
- the horizontal axis is the time (in seconds).
- Figure 8 is a view to view the temperature dependence of the calculation result of S0 3 generation concentration on HN0 3 addition amount.
- the horizontal axis is temperature (K)
- the vertical axis represents S0 3 concentration (ppm).
- S0 2 concentration in the combustion gas is 2000 p pm
- the HN0 3 concentration 1 00 ppm
- 200 p pm 1 000 ppm
- conditions other than those varied are the same as in FIG.
- FIG. 9 is a diagram showing a configuration of a vacuum treatment apparatus for use in desulfurization and denitration method of combustion gases containing S0 2 and NO gas by HN0 3 addition.
- a decompression processing device 10 includes a vacuum chamber 11, a reaction tube 12 which is provided so as to penetrate the vacuum chamber 11 and is supplied with combustion gas, and a heating tube for heating the reaction tube 12. It comprises a heater 13, a combustion gas supply sound 15, a combustion gas exhaust section 16, and a mass spectrometer 20.
- the reaction tube 12 is provided so as to penetrate the vacuum chamber 11.
- a combustion gas supply unit 15 is connected to the end 12 a of the external reaction tube in the vacuum chamber 11, and a combustion gas exhaust unit 16 is connected to the other end 12 b of the external reaction tube in the vacuum chamber 11 1
- a pinhole 12 c for discharging the combustion gas to the vacuum chamber 11 is provided at the center thereof.
- the reaction tube 12 is heated to a reaction temperature of 600 K to 80 OK by a heater 13 such as a ribbon heater.
- the temperature of the reaction tube 12 is measured by a thermocouple 14 movably installed inside the reaction tube 12, and the temperature of the heater 13 is controlled by a temperature controller (not shown).
- reaction tube 12 a quartz glass reaction tube with an inner diameter of 1.5 cm and a length of 60 cm coated with boron glass (B 2 ⁇ 3 ) on the inner wall was used, and the pinhole diameter was , 0.1 mm.
- the temperature distribution in the center of the reaction tube has a soaking area of 15 cm within a range of ⁇ 5.
- a typical total flow is 100 sccm.
- sc cm standard cubic cm per minute: cm 3 / min
- the residence time in the high-temperature reactor is from 0.1 second to 0.5 seconds.
- the pressure of the combustion gas is measured by a vacuum pressure gauge 17 and, for example, a capacitive pressure gauge (trade name: Baratron) can be used.
- the lower limit of the above reaction tube pressure is determined by the condition that the sampling from the pinhole portion 12 c of the reaction tube to the mass spectrometer 20 is a molecular beam
- the upper limit of the reaction tube pressure is It is determined by the performance of the exhaust system. Due to these limitations, the measurement conditions of the reaction product measurement device 10 are ones in which the pressure is significantly lower than the actual exhaust gas conditions from the combustor.
- the mass spectrometer 20 uses a quadrupole mass spectrometer (Anelva AQA400).
- a combustion gas introduction hole 20a having a diameter of 1 mm provided at the tip is inserted into the inside of the vacuum chamber 11 and faces the pinhole section 12a of the reaction tube 12.
- the combustion gas flowing into the combustion gas introduction hole 20a from the pinhole portion 12a of the reaction tube 12 is differentially exhausted by a differential exhaust device 21 using a turbo molecular pump or the like, and the mass spectrometer 20 To the ionization chamber.
- the combustion gas guided to the ionization chamber is ionized by an electronic impulse.
- the mass-selected ions are detected by a secondary electron multiplier, and the data processing device displays the calculated data.
- the decomposition of the combustion gas due to ionization that is, if fragmentation occurs, the analysis of the combustion gas cannot be performed accurately. Therefore, in order to suppress fragmentation, the ionization energy was set to a minimum of 10 eV to 30 eV so as not to decompose the reaction gas.
- the vacuum chamber 11 is evacuated by an evacuation device 18.
- the evacuation device 18 includes a vacuum pump including an opening / closing gate valve, an oil rotary pump, a turbo-molecular pump, and a vacuum gauge. It consists of a control device for evacuation.
- the vacuum chamber 11 of the decompression processing apparatus 10 was evacuated to a predetermined degree of vacuum, and the reaction tube was heated to 600 to 800 K by the heater 4 .
- the reaction tube was heated to 600 to 800 K by the heater 4 .
- the Eta 2 as the total pressure, the 1 0 ⁇ ⁇ ⁇ ⁇ 8 0 ⁇ ⁇ ⁇ ⁇ ⁇ Flow from the combustion gas supply section to the reaction tube.
- the reaction temperature is in the 6 0 0 ⁇ 80 0 ⁇ , S0 3 production was observed by the mass spectrometer.
- Figure 1 0 is a view showing a HN_ ⁇ 3 amount dependent S_ ⁇ 3 generation amount of 7 5 0 K in the vacuum processing apparatus of FIG.
- the vertical axis represents the mole fraction of S_ ⁇ 3 (in arbitrary scale of X 1 0 0 0 0)
- the horizontal axis represents the HN_ ⁇ third pressure that is added to the reaction tube (the To rr).
- the black circles are the measured values
- the solid lines are the values calculated by simulation described later. It is.
- the pressures of the combustion gases S0 2 , 0 2 , N ⁇ , H 2 , and N 2 are 1.0 Torr, 50.0 Torr, 0.2 To rr, 0.05 Torr, and approximately 29 Tor, respectively. r.
- the pressure of the No. 2 gas is a carrier gas when the No. 3 is introduced, and fluctuates according to the No. 3 pressure.
- the total pressure is 81 Torr.
- reaction gas pressure is in a low pressure of about 1/10 of the atmospheric pressure, conversion to S_ ⁇ 3 S0 2 in such a low pressure, the lower than atmospheric pressure of the simulation Conceivable.
- reaction (R 1) is a three-molecule reaction in the pressure fall-off region, and the reaction rate decreases as the pressure decreases.
- Desulfurization and denitrification method S_ ⁇ 2 and NO in the combustion gases according to the present invention is constructed as above, as described above, the S_ ⁇ 2 and NO in the combustion gas containing oxygen, 6 00K ⁇ by adding at a relatively low temperature ⁇ _Ita radical 800 kappa, by rise to chain reaction, it can be treated by simultaneously oxidized to S0 3 and N_ ⁇ 2.
- OH radicals can be generated by nitric acid.
- the present invention is not limited to the above embodiments, and various modifications are possible within the scope of the invention described in the claims, and it goes without saying that they are also included in the scope of the present invention. .
- the pressure of the combustion gas containing S 0 2 and NO explained in the above embodiments that may be atmospheric pressure as a matter of course. It is also apparent that the method of the present invention can be easily applied to various types of combustion devices. Industrial applicability
- the present invention can realize a desulfurization and denitration method capable of simple desulfurization of S 2 and denitration of NO by adding a H radical. This method is easy to configure and low cost.
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Abstract
La présente invention a trait à un procédé de réalisation de désulfuration de SO2 et de dénitrification de NO, le SO2 et le NO étant présents dans un gaz de combustion produit dans un procédé de combustion, comprenant l'ajout d'un radical OH au gaz de combustion, pour produire une réaction en chaîne et l'oxydation de SO2 et de NO simultanément. Dans un mode de réalisation, on ajoute du HNO3 (acide nitrique) au gaz de combustion pour générer un radical OH. On peut ajouter un gaz M inerte à la réaction au gaz de combustion. De préférence, la procédé de combustion est effectué à la pression atmosphérique à une température comprise entre 600 K et 800 K. Ce procédé permet la désulfuration et la dénitrification aisée, simple et économique par voie sèche sans catalyseur.
Applications Claiming Priority (2)
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JP2003-54899 | 2003-02-28 | ||
JP2003054899A JP3879102B2 (ja) | 2003-02-28 | 2003-02-28 | So2及びnoの酸化方法 |
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WO2004076035A1 true WO2004076035A1 (fr) | 2004-09-10 |
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PCT/JP2003/015610 WO2004076035A1 (fr) | 2003-02-28 | 2003-12-05 | Procede de realisation de desulfuration et de denitrification |
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WO (1) | WO2004076035A1 (fr) |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN100427180C (zh) * | 2007-01-26 | 2008-10-22 | 昆明理工大学 | 一种用生物质热解气还原低浓度二氧化硫的方法 |
CN101961596A (zh) * | 2010-07-19 | 2011-02-02 | 大连海事大学 | 氧活性粒子注入烟道中的羟基自由基氧化脱硫脱硝方法 |
Families Citing this family (1)
Publication number | Priority date | Publication date | Assignee | Title |
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JP4596947B2 (ja) * | 2005-03-25 | 2010-12-15 | 財団法人石油産業活性化センター | 水硫化アンモニウム環境下における材料の耐腐食性評価方法 |
Citations (9)
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JPS5162180A (ja) * | 1974-11-29 | 1976-05-29 | Mitsubishi Heavy Ind Ltd | Shitsushikihaienshorihoho |
JPS52138053A (en) * | 1976-05-14 | 1977-11-17 | Mitsubishi Heavy Ind Ltd | Removal of nitrogen oxide in exhaust gas |
WO1992020433A1 (fr) * | 1991-05-21 | 1992-11-26 | Institute Of Nuclear Chemistry And Technology | PROCEDE D'EXTRACTION DE SO2 ET DE NOx DE GAZ DE COMBUSTION ET INSTALLATION UTILISEE A CET EFFET |
JPH05161821A (ja) * | 1991-12-16 | 1993-06-29 | Senichi Masuda | 排ガス処理方法 |
JPH0731844A (ja) * | 1993-07-26 | 1995-02-03 | Ebara Corp | 脱硝・脱硫副生物の付着防止方法 |
JPH07256056A (ja) * | 1994-03-23 | 1995-10-09 | Toshiba Corp | 廃棄物質の処理方法 |
JPH08243340A (ja) * | 1995-03-13 | 1996-09-24 | Mitsui Eng & Shipbuild Co Ltd | 排ガス処理装置及び方法 |
JPH09299762A (ja) * | 1996-05-10 | 1997-11-25 | Toshiba Corp | 排ガス処理システム |
JP2000117049A (ja) * | 1998-08-10 | 2000-04-25 | Sandensha:Kk | 窒素酸化物・硫黄酸化物の浄化方法及び浄化装置 |
-
2003
- 2003-02-28 JP JP2003054899A patent/JP3879102B2/ja not_active Expired - Fee Related
- 2003-12-05 WO PCT/JP2003/015610 patent/WO2004076035A1/fr active Search and Examination
Patent Citations (9)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JPS5162180A (ja) * | 1974-11-29 | 1976-05-29 | Mitsubishi Heavy Ind Ltd | Shitsushikihaienshorihoho |
JPS52138053A (en) * | 1976-05-14 | 1977-11-17 | Mitsubishi Heavy Ind Ltd | Removal of nitrogen oxide in exhaust gas |
WO1992020433A1 (fr) * | 1991-05-21 | 1992-11-26 | Institute Of Nuclear Chemistry And Technology | PROCEDE D'EXTRACTION DE SO2 ET DE NOx DE GAZ DE COMBUSTION ET INSTALLATION UTILISEE A CET EFFET |
JPH05161821A (ja) * | 1991-12-16 | 1993-06-29 | Senichi Masuda | 排ガス処理方法 |
JPH0731844A (ja) * | 1993-07-26 | 1995-02-03 | Ebara Corp | 脱硝・脱硫副生物の付着防止方法 |
JPH07256056A (ja) * | 1994-03-23 | 1995-10-09 | Toshiba Corp | 廃棄物質の処理方法 |
JPH08243340A (ja) * | 1995-03-13 | 1996-09-24 | Mitsui Eng & Shipbuild Co Ltd | 排ガス処理装置及び方法 |
JPH09299762A (ja) * | 1996-05-10 | 1997-11-25 | Toshiba Corp | 排ガス処理システム |
JP2000117049A (ja) * | 1998-08-10 | 2000-04-25 | Sandensha:Kk | 窒素酸化物・硫黄酸化物の浄化方法及び浄化装置 |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN100427180C (zh) * | 2007-01-26 | 2008-10-22 | 昆明理工大学 | 一种用生物质热解气还原低浓度二氧化硫的方法 |
CN101961596A (zh) * | 2010-07-19 | 2011-02-02 | 大连海事大学 | 氧活性粒子注入烟道中的羟基自由基氧化脱硫脱硝方法 |
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Publication number | Publication date |
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JP3879102B2 (ja) | 2007-02-07 |
JP2004263946A (ja) | 2004-09-24 |
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