• 专利附录
  • 专利说明
  • 权利要求
  • 类似技术
  • 同族专利
  • 引用文献
  • 法律状态
  • 优先权
    • 专利摘要:
    A process to produce sulphur from two acid gases both containing hydrogen sulphide and one of which contains ammonia, using a modified Claus technique. The acid gas containing ammonia is burnt in the presence of air under substoichiometric conditions in a first heat-reaction chamber, while the ammonia-free acid gas is burnt in a second heat-reaction chamber, forming a series with the first chamber, with the right quantity of air to provide a molar ratio of H2S to SO2 of approximately 2/1 at the catalytic reaction stage inlet. The mixed effluents from both heat-reaction chambers may pass through a high-temperature residence chamber before being conveyed to the heat-recovery stage. Gas effluents from the heat-reaction stage contain H2S and SO2 in the right ratio for the catalytic reaction stage, and no hydrocarbons or harmful quantities of NH3 and NO.
    公开号:SU974934A3
    申请号:SU792762795
    申请日:1979-04-28
    公开日:1982-11-15
    发明作者:Деграншан Ги；Квасникоф Жорж；Блан Клод
    申请人:Сосьете Насьональ Елф Акитэн (Продюксьон) (Фирма)；
    IPC主号:
    专利说明:

    one
    The invention relates to methods for producing sulfur from two acid gases, one of which contains mainly hydrogen sulfide, and the other ammonia and hydrogen sulfide or one ammonia.
    At oil refineries, there are usually two acidic hydrogen sulfide gases, one of which mainly contains hydrogen sulfide, a few percent of hydrocarbons and does not contain ammonia, and the second does not contain hydrocarbons and, in addition to H, 5 contains ammonia 2% by volume.
    Thus, the sour gas, including the MNZ, contains 93% by volume, 2% by volume of hydrocarbons and 5% of water, while the ammonia acid contains 6% by volume | 30 vol%, 30 vol%, HH ,, and 40 vol% NZO, the ammonia acid gas containing cannot be processed according to the traditional Claus method without special precautions, because the molar ratio must be maintained in this process: SOs close to 2: 1 in gases coming from the term of term 25
    This reaction leads to combustion conditions such that the temperatures reached are not sufficient to ensure proper destruction. It is known that even small amounts of unburned agglomerate in gases leaving the thermal reaction leads to the inevitable deposition of ammonium salts in some parts of the installation which can lead to jamming communications.
    A method is known for producing sulfur from acid gases containing hydrogen sulfide and appreciable amounts of ammonia, in which the ammonia gas is subjected to an operation to remove the ammonia contained in it before feeding the specified acid gas to the Claus process unit. The essence of the method lies in the fact that the ammonia gas is first displaced with an acid gas not containing ammonia, preheated sufficiently so that the mixture of two acid gases has a temperature of at least 70 ° C, in particular about 8 ° C, indicated in the examples, in order to avoid the occurrence of solid deposits of ammonium salts, said mixture I31 is jetted at this temperature into the burner located at the inlet to the stage of the thermal reaction of the Claus unit to the indicated burner, moreover, the air needed to oxidize sub-ammonia to nitrogen and to carry out the mixed oxidation of hydrogen sulphide to sulfuric anhydride in order to obtain a molar ratio of close to 2: 1 in the gases leaving the thermal reaction stage 1. The disadvantage of this method is that the acidic ammonia gas is mixed with the ammonia-free acid gas before the thermal reaction step. In addition, combustion conditions associated with the need to obtain a molar ratio of: SO close to 2: 1 in the gases released after combustion are such that the temperature reached is not sufficient to ensure satisfactory removal of ammonia, and it is important that the various walls of the plant, when in contact with the gas obtained as a result of combustion, were maintained above 150 ° C to avoid the formation of solid deposits of ammonium salts due to the presence of unburned ammonia in gases from the game. The closest to the proposed technical essence and the achieved result is the method consisting in the fact that the combustion of the source gas is carried out in two stages: with ISSO-ISSO C in the first and 1000-1500 in the second. The essence of the method is that an acidic ammonia gas mixed with a part of the ammonia-free gas is injected into the burner at the entrance to the first thermal reaction zone, and the entire amount of air required for the complete combustion of ammonia to nitrogen is fed into the burner. and mixed oxidation of hydrogen sulphide to sulfuric anhydride to obtain a H2: S ratio of 2: 1 in gases from the thermal reaction stage, while ammonia-free acid gas, its remaining part is introduced into the BToiiyra zone term chesky reaction, razmeyshe gay nale the first zone Under these conditions, as a result of the oxidation of a significant amount of hydrogen sulfide into sulfuric anhydride, an elevated temperature is established in the first thermal reaction zone 44, which favors the decomposition of ammonia. Adding an acid gas that does not contain ammonia, injected into the second thermal reaction zone, then allows the molar ratio of H j S: S O 2 ak to be corrected so that it is close to 2: 1 in the gases leaving the thermal reaction stage. The known method is caused by the presence of quasi-stable (-, hydrocarbons in an acidic gas that does not contain ammonia. Hydrocarbons present in the specified acidic gas injected into the second thermal reaction zone do not find the oxygen required for their combustion, and therefore, they are not removed, which leads to coking of the catalysts at the stage of catalytic reaction with a decrease in the activity of these catalysts and coloring of the sulfur product.The purpose of the invention is to ensure that the acid gases containing hydrocarbons can be processed without coking of the catalyst. the first stage is subjected to burning ammonia-containing sulfuric hydrogen gas with an air flow rate of 6 °, .5-1, and to the second - hydrogen sulfide gas is burned with this amount of air, To the outlet from the thermal stage gas has a molar ratio: SO, 2: 1. In addition, at a molar ratio contained in the gas supplied to the second stage of combustion, to in the gas supplied to the first stage equal to or greater than 2, air to the first stage of combustion is supplied with a flow coefficient of 0.7-1. .When the molar ratio H S is contained in the gas supplied to the second stage, and in the gas entering the first stage is less than 2, air is supplied to the first stage with a flow coefficient of 0.5-O, 7, and the source gas and air are preheated to 15O-250C. Preliminary; the gases are heated by indirect heat exchange with the steam obtained in the combustion stage. Gases before the cooling stage are held at 1000–1500 ° C for 0.2–1.2 s. The choice of the above conditions is due to the fact that, with the proposed parameters, the content of NVl in the gas flowing out of the thermal reactor is less than 5 Ofr, which eliminates the formation of ammonium salt deposits. The drawing shows a schematic diagram of an installation for carrying out the method according to the invention. The installation includes a thermal reactor 1 having first and second thermal reaction chambers 2 and 3, respectively, and a gas extraction chamber 4 at an elevated temperature, the said refractory material chambers are arranged in series and are connected each with intermediate partitions 5 and 6 of refractory material. The first thermal reaction chamber is equipped with an axial burner 7 equipped with a nozzle 8 for supplying the first acid gas, i.e. ammoniaic acid gas, and a pipe 9 for supplying air. The second thermal reaction chamber is provided with a radial burner 10 entering the said chamber near the cellular partition 5, equipped with a nozzle 11 supplying a second acid gas, i.e. sour gas that does not contain ammonia and the pipe 12, which supplies air. Exit from the thermal reactor, i.e. The exit from the last thermal reaction chamber of the specified reactor, connected by a pipe 13 with a thermal waste-heat boiler 14, is operated by indirect heat exchange: to generating steam from water introduced through pipeline 15, steam is removed through a pipe 16. At the exit of the heat recovery boiler a condenser 17 for separating sulfur is located, the indicated condenser is equipped with a pipe 18 for removing liquid sulfur. The output from the condenser is connected to the entrance to the catalytic reaction stage 19. The latter usually consists of two or three catalytic chambers arranged in the form of a battery, each of which has a preheater for the gas mixture being treated, and after them there is a condenser for separating sulfur. The condenser 2O, following the last catalytic chamber, has a pipe 21 for the removal of liquid sulfur. An afterburner 22 is placed after the condenser, which is connected to the exhaust pipe 23. To maintain the temperature in the first thermal reaction chamber at the desired level, affect the cost ratio of ammonia gas and air introduced into the first thermal reaction chamber through the burner 7, and On the other hand, to maintain the molar ratio: Qy equal to or close to 2: 1 at the inlet to the catalytic stage, the ratio between the flow rates of the acid gas not containing ammonia and the air introduced into the second chamber is minutes of reaction through the burner 10, used are known in the art and the control means control (not shown). The method is carried out as follows. The acidic ammonia gas is fed to the burner 7 through the pipe 8, while the corresponding amount of air is transferred to the pipe 9. The combustible mixture prepared in this way is burned and the gases obtained from burning the ammonia gas are 0.2-1.2 c are in the thermal reaction chamber 2 (the first chamber) before entering the thermal reaction chamber 3 (the second chamber) through the cell wall 5. The temperature in the thermal reaction chamber 2 is controlled at the level selected between 1350-1550 ° C, affecting the flow ratio sour ach--gas and air fed into this chamber. Ammonia sour gas and its corresponding air can be injected into the thermal reaction chamber 2 either without preheating or after preheating up to 15O-250C. The acid gas, which does not contain ammonia, is fed to the burner 10 through the pipe 1 1, while the required amount of air corresponding to obtaining the molar ratio I-L S:; S02, blistering; to 2: 1 in the combustion gases at the exit to the catalytic reaction stage, is fed through nozzle 12 to the colder space of chamber 3. The combustible mixture thus obtained is burned and the gases from burning ammonia-free acid gas are mixed in the thermal reaction chamber 3 (the second chamber thermal reaction) with combustion gases leaving chamber 2, the residence time in chamber 3 of the mixture of combustion gases thus obtained from 0.2-1.2 s. This mixture passes through a cellular partition 6, which improves the quality of this mixture, it is still 0.2-1.2 s in chamber 4, at an increased temperature, in which the temperature is still higher. The reaction mixture leaving the thermal reactor is subjected to the first cooling in the term „7S7 heat recovery boiler 14, then it is cooled more strongly in the condenser 17, where part of the sulfur contained in the indicated reaction mixture is condensed, sulfur can be diverted through pipe 18. Reaction the mixture leaving the condenser 17 is then sent after a preheating; 1 n preheating to the catalytic conversion stage for converting to sulfur those quantities of hydrogen sulfide and sulfur dioxide that are still contained in it. At the exit from the catalytic conversion stage, the gas mixture enters the condenser .20 to separate the sulfur, then to the afterburner 22 to convert to sulfurous anhydride. The last traces of sulfurous compounds are released before the atmosphere through the exhaust pipe 23. The molar ratio is 6O2. at the entrance to the catalytic conversion stage, it is maintained at approximately 2: 1 or close to that value, influenced by the ratio of the flow rates of the acid gas that does not contain ammonia and air introduced into the thermal reaction chamber 3. In the thermal reaction chamber 2 (the first thermal reaction) burning of acidic ammonia gas is carried out under reducing conditions (such that the molar ratio of HoS: SO in the gases leaving ife of this chamber is less than or equal to 2) in order to minimize or even avoid the formation of NO, and besides slave The temperature setting in this chamber (135 O-ISSO C) leads to a high decomposition rate of ammonia. The radial or tangential burner located in the thermal reaction chamber 3 (the second thermal reaction chamber) is supplied with an acid gas that does not contain ammonia, this gas is usually an acid gas with a high content of hydrogen sulfide, and the air flow is such that the molar ratio O, in the waste gases after combustion, entering the inlet of the catalytic reaction stage, was close to 2: 1. Hydrocarbons present in an acid gas that does not contain ammonia are burned in the thermal reaction chamber 3 as a result of a supply of oxygen and high temperatures that develop in this chamber. Traces of non-combustible ammonia in gases, extracted from the thermal reaction chamber 2 (residence time 0.2–1.2 s), take place in chamber 3 of the thermal reaction under conditions favorable to their decomposition. Following this, gas removal improves. . In addition, traces of MO, which can form in the thermal reaction chamber 2, are removed under severely reducing conditions at elevated temperature, which are created in the thermal reaction chamber 3. The passage of flue gases from the combustion of two acidic gases, ammonia and not containing ammonia, through The staying chamber 4 at a higher temperature before they are cooled in the recovery boiler makes it possible to further improve the mixture of said exhaust gases and decompose the last traces of ammonia and UO that may still be contained in it. At the exit from the thermal reaction stage carried out in accordance with the invention, the gases leaving after combustion do not contain any more interfering amounts of ammonia, MO and SO. Example 1. The experiments were carried out to obtain sulfur from two acid gases, one of which is ammonia and contains,% by volume, ammonia 30, hydrogen sulfide 30 and water 40, and the second gas does not contain ammonia and contains,% vol. Hydrogen sulfide 92, hydrocarbons 2.5 and water 5.5. They operate at a facility similar to that described using a thermal reactor containing two thermal reaction chambers and a gas residence chamber at elevated temperature. Sour ammonia gas and combustion air are fed to the burner of the first thermal reaction chamber without preheating and with molar flow rates of 2O and 51.4 mol / h, respectively, the amount of air used corresponds to a value of 0.8. The temperature in the first thermal reaction chamber is set to approximately 1450 ° C. An acidic gas that does not contain ammonia and the corresponding air for its combustion is fed into the burner of the second thermal reaction chamber with molar flow rates, respectively, equal to 33 and 57.3 mol / h, which leads to a value close to 2: 1, for the molar ratio HS: BO 7. at the entrance to the catalytic reaction zone. The temperature in the second thermal reaction chamber is about 12. The gas streams after the combustion of an oxygen-free acid gas, combined with the off-gases after the combustion of an acid ammonia gas, then pass through the gas confinement zone (third chamber) at 1230 ° C before they are sent to the waste heat boiler. Time
    the residence of the combustion gases in each of the thermal reaction chambers is approximately 0.5 s.
    Ammonia, NO and hydrocarbon content, expressed in volumes per million
    (abbreviated as omd) in the exhaust gases from each chamber (first and second) of the thermal reaction and the chamber (third) of the gas are shown in the table.
    NHo,
    N0 Hydrocarbons In the gases coming from the first thermal reaction chamber, the presence of unburned ammonia is noted, as well as insignificant amounts of NO, which is formed despite the substoichiometric burning conditions existing in this chamber. In the gases entering the second thermal reaction chamber, only the presence of very small amounts (approximately 68 ám) of unburned ammonia and melt (about 12 ám) N0 is noted. The analysis of the exhaust gases from the residence chamber indicates that the reduction of NO 0 is still ongoing in this last chamber (approximately 6 ohm NOB exhaust gases). After 700 hours of operation, no deposits are observed on the walls of parts of the plant when they come into contact with gases passing after the thermal reactor, Example 2. Work on the plant, as in Example 1, is carried out to obtain sulfur from two acid gases, one of which is ammonia and contains, vol.%, ammonia 30, hydrogen sulfide 30 and water 40, and the other does not contain ammonia and contains, vol%, hydrogen sulfide 82, hydrocarbons 2.5 and water 5.5. Sour ammonia gas and its combustion air, prior to 5 but heated to 210 ° C, are fed into the burner of the first thermal reaction chamber with polar consumption equal to 29 and 56.7 mop / h, respectively, the amount of air used is 0.5. The temperature in the first thermal chamber, the reaction is set to 136СРС. Acidic gas which does not contain ammonia K) and the air for its combustion are fed to the burner of the second chamber by thermal reaction with molar flow rates, respectively
    68
    45 6
    12
    权利要求:
    Claims (5)
    [1]
    It is not definitively equal to 16.5 and 49.5 mol / h in order to obtain a molar ratio in gases at the entrance to the catalytic reaction zone, close to 2: 1. The temperature in the second thermal reaction chamber is% 1400С. The gases released after burning the ammonia-free acid gas, combined with the gases from the combustion of the acid ammonia gas, then pass through the gas dwelling zone at a temperature of 1400 ° C before they are sent to the waste-heat boiler. The residence time of the gas in each of the thermal reaction chambers and the gas residence chamber is approximately 0.5 s. The analysis of the gases leaving the residence chamber does not show any harmful amounts of ammonia, NO and SOy. Also, no soot deposition is observed on the catalysts. in the catalytic reaction zone. Claim 1. Method for producing sulfur from two hydrogen sulfide gas streams, one of which contains hydrogen sulfide and ammonia, and the other only hydrogen sulfide, which includes thermal source gas in two stages at 1350-1550 ° С on the first one and lpOO-1500 С on the second, subsequent cooling of the combustion products and their processing at catalytic stages, characterized in that, in order to enable the processing of hydrocarbon-containing gases and prevent catalyst coking, in the first stage, Ammaxo is subjected to combustion; Hydrogen sulfide; Nitrogen gas with an air flow rate of ot 0.5–1, and in the second stage hydrogen sulfide gas is burned with such a quantity of air that at the exit from the Thermal stages the gas has a molar ratio of 0: 2: 1.
    [2]
    2. The method according to claim 1, wherein the molar ratio of Hife I contained in the gas supplied to the second stage of combustion to the HiS in the gas entering the first stage is equal to or greater than 2, air is fed to the first combustion stage with a flow ratio of 0.7-1,
    [3]
    3. The method according to claim 1, of which is with Tpvj, that at the molar ratio of the scientific research institute, “which is concentrated in the gas supplied to the second stage, and in the gas supplied and the first stage, less than 2 , air to the first stage is served with
    lg fl
    sh
    J 9
    and 4, with a flow coefficient of 0.5-O, 7, where the source gas and air are preheated to 15 O-250 C ,.
    [4]
    4. The method of claim 3, wherein the preheating of the gases is carried out by indirect heat exchange with the steam obtained in the cooling phase of the gases leaving the burning stage.
    [5]
    5. The method according to claim 1, characterized in that the gases before the cooling stage are kept at 10001500 ° C for 0.2-1.2 s. information taken into account in the examination 1.Patent of France No. 2247421, cl. C 01 B 17/04, 1974. 2. US patent number 3970743, l. C O1 17/04, 1976.
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    同族专利:
    公开号 | 公开日
    NL188746B|1992-04-16|
    CA1119386A|1982-03-09|
    GB2019827A|1979-11-07|
    US4596699A|1986-06-24|
    NL188746C|1992-09-16|
    NL7903412A|1979-11-06|
    DE2917245C2|1996-03-07|
    GB2102692A|1983-02-09|
    GB2102692B|1983-06-02|
    FR2424875B1|1981-08-14|
    GB2019827B|1983-02-02|
    US4395390A|1983-07-26|
    DE2917245A1|1979-11-15|
    FR2424875A1|1979-11-30|
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    DE2537451C2|1975-08-22|1987-05-27|Carl Still Gmbh & Co Kg, 4350 Recklinghausen|Process for converting the ammonia contained in coke oven gases into nitrogen and water and the hydrogen sulfide into sulfur|EP0034848B1|1980-02-26|1984-04-18|Shell Internationale Researchmaatschappij B.V.|A process for combusting ammonia-containing gases which also contain hydrogen sulphide|
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    DE3639156A1|1986-11-15|1988-05-26|Basf Ag|TRISAZO DYES|
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    US4994242A|1988-08-15|1991-02-19|Noram Engineering And Constructors Ltd.|Jet impingement reactor|
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    法律状态:
    优先权:
    申请号 | 申请日 | 专利标题
    FR7812899A|FR2424875B1|1978-05-02|1978-05-02|
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