JP3646885B2 - Removal of hydrogen sulfide from gas streams - Google Patents

Removal of hydrogen sulfide from gas streams Download PDF

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JP3646885B2
JP3646885B2 JP33756594A JP33756594A JP3646885B2 JP 3646885 B2 JP3646885 B2 JP 3646885B2 JP 33756594 A JP33756594 A JP 33756594A JP 33756594 A JP33756594 A JP 33756594A JP 3646885 B2 JP3646885 B2 JP 3646885B2
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hydrogen sulfide
gas stream
catalytic reactor
catalytic
sulfur
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JPH08183972A (en
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サンデル・ステゲンガ
アントニウス・マリア・デムメルス
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Shell Internationale Research Maatschappij BV
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Description

【０００１】
【産業上の利用分野】
本発明は、ガス流からの硫化水素の除去方法に関するものである。この種のガス流の例は天然ガスである。
【０００２】
【従来の技術】
国際特許出願第９２／０２ ４４９号公報にはガス流からの硫化水素の除去方法が記載され、この方法はガス流を元素硫黄の露点よりも高い温度で遊離酸素の存在下に第１接触反応器で触媒材料と接触させて部分精製されたガス流を得ると共に、この部分精製されたガス流を水の露点と元素硫黄の露点との間の温度にて第２接触反応器で触媒材料と接触させて精製ガス流を得ることからなっている。
この公知方法においては、空気を第１接触反応器の上流にてガス流に供給する。空気中の遊離酸素は硫化水素を次の反応：
Ｈ2 Ｓ＋１／２ Ｏ2 −−−−−＞Ｈ2 Ｏ＋１／ｘ Ｓx
にしたがい元素硫黄まで直接に酸化する。
前記特許公報は第１接触反応器に供給される遊離酸素の量につき黙しているが、この量は一般に化学量論量または僅かに化学量論量より大である。すなわち、酸素と硫化水素との濃度間の比は０．５、すなわち化学量論比またはそれ以上である。この比の単位は標準圧力および温度にてモル／モルもしくはｖｏｌ／ｖｏｌである。本明細書においては、酸素と硫化水素との濃度間の比を「酸素−硫化水素の比」と称する。
【０００３】
今回、本出願人はガス流を第１接触反応器にて水の露点と元素硫黄の露点との間の温度で元素硫黄が第１接触反応器における触媒材料に吸着されるよう触媒材料と接触させることを提案する。この第１接触反応器は硫化水素を大量除去すべく用いられ、第２接触反応器は第１接触反応器より流出するガスから微量の硫化水素を除去すべく使用される。
本発明の方法においては第１接触反応器を用いてガス流から多量の硫化水素を除去し、したがって生成する元素硫黄の大部分がこの接触反応器における触媒材料に吸着される。吸着された元素硫黄は触媒材料の活性を増大させる。しかしながら、触媒材料に吸着される元素硫黄の量が所定レベルよりも高ければ、硫化水素の変換率が低下し、これは触媒材料に吸着される硫黄の量と共に低下する。したがって、より多量の硫化水素が第１接触反応器から流出する。硫化水素の漏れを減少させるには、第１接触反応器における触媒材料をＨ2 Ｓ変換率が所定レベル以下に低下する前に再生せねばならない。したがって、順次の２回の再生の間における時間は、Ｈ2 Ｓ変換率が所定レベル以下に低下した第１接触反応器における硫黄量に達するのに要する時間により決定される。
【０００４】
【発明が解決しようとする課題】
本発明の課題は、サイクル時間を増大させることにある。
【０００５】
【課題を解決するための手段】
上記課題を解決すべく、本発明によるガス流からの硫化水素の除去方法は、ガス流を遊離酸素の存在下に水の露点〜元素硫黄の露点の範囲の温度にて２個の接触反応器で触媒材料と接触させて触媒材料に沈着する元素硫黄と精製ガス流とを得、ガス流を第１接触反応器にて触媒材料と化学量論量未満の遊離酸素の存在下に接触させて部分精製されたガス流を得、この部分精製されたガス流を第２接触反応器にて追加遊離酸素の存在下に触媒材料と接触させて精製ガス量を得ることからなっている。
本発明は、Ｈ2 Ｓ−変換率が低下する触媒材料の硫黄量は酸素−硫化水素の比に依存すると言う知見に基づいている。この比が０．５より大またはそれに等しければ初期Ｈ2 Ｓ−変換率は一般に９５〜１００％になるが、Ｈ2 Ｓ−変換率が低下し始める触媒材料の硫黄量は４０％未満である。酸素−硫化水素の比が０．５未満になればＨ2 Ｓ−変換率は９５％未満になるが、Ｈ2 Ｓ−変換率が低下し始める触媒材料の硫黄量は酸素−硫化水素の比が０．５もしくはそれ以上である際にＨ2 Ｓ−変換率が低下し始める硫黄量の約２倍であることが判明した。この作用を以下の例で示す
【０００６】
Ｈ2 Ｓ−変換率を触媒材料における硫黄量の関数として決定すべく３種の実験を行った。これら実験では水で飽和された窒素流を用いて、水で飽和されたメタン流をシミュレートした。窒素流はさらに１容量％のＨ2 Ｓと１容量％のＣＯ2 と２００ｐｐｍｖ（１，０００、０００分の１容量部）のＣＯＳと遊離酸素とを含有した。遊離酸素の量を、酸素−硫化水素の比が０．６、０．４５および０．２７となるよう選択した。［Ｏ2 ］対［Ｈ2 Ｓ］の化学量論比は０．５である。使用した触媒材料は活性化アルミナ触媒（ラ・ロッシュ社からのＡ２０１）とした。圧力は１０バールとし、温度は１５０℃とし、ガス空時速度は２ ０００ｖｏｌ／ｖｏｌ／ｈｒとした。表１には各実験の結果を、変換率が酸素−硫化水素比の関数として低下し始める際の触媒の初期Ｈ2 Ｓ−変換率および硫黄量として示す。初期Ｈ2 Ｓ−変換率は１−［Ｈ2 Ｓ］out ／［Ｈ2 Ｓ］in（ここで［Ｈ2 Ｓ］inは接触反応器に流入するガス流における硫化水素の濃度であり、［Ｈ2 Ｓ］out は接触反応器から流出するガス流における硫化水素の濃度である）として規定される。触媒の硫黄量は触媒１ｋｇ当りの硫黄ｋｇとして現わす。
【０００７】
【表１】

Figure 0003646885
【０００８】
好適には第１接触反応器中へ流入するガス流における本発明の方法の酸素−硫化水素比は０．４０〜０．４９の範囲、より好ましくは０．４５〜０．４９の範囲である。
第２接触反応器は微量の硫化水素を除去すべく使用され、この目的で部分精製れたガス流を第２接触反応器にて追加遊離酸素の存在下に触媒材料と接触させる。追加遊離酸素の量は、ガス流中に存在する硫化水素の初期量と共に酸素の全量が化学量論量に等しく或いはそれより大となるよう選択される。
【０００９】
以下、本発明による方法を実施するための装置を示す添付図面を参照して、実施例により本発明を一層詳細に説明する。
装置は参照符号１、２および３で示す触媒材料を内蔵する３個の反応器と、供給物の供給導管４と、精製ガスの出口導管５と、再生ガスの供給導管６と、硫黄含有ガスの出口導管７と、凝縮器８と、硫黄の貯蔵タンク９と、接続導管１０とで構成される。
各接触反応器１、２および３は参照符号１５、１６および１７で示す下側マニホールドを有する。下側マニホールド１５は弁１５ａ、１５ｂおよび１５ｃを導管１５ｄ、１５ｅおよび１５ｆに備え、下側マニホールド１６は弁１６ａ、１６ｂおよび１６ｃを導管１６ｄ、１６ｅおよび１６ｆに備え、さらに下側マニホールド１７は弁１７ａ、１７ｂおよび１７ｃを導管１７ｄ、１７ｅおよび１７ｆに備える。導管１５ｄ、１６ｄおよび１７ｄは供給物の供給導管４に接続され、導管１５ｅ、１６ｅおよび１７ｅは精製ガスの出口導管５に接続され、さらに導管１５ｆ、１６ｆおよび１７ｆは再生ガスの供給導管６に接続される。
【００１０】
さらに各接触反応器１、２および３は参照符号２０、２１および２２で示す上側マニホールドをも備える。上側マニホールド２０は弁２０ａおよび２０ｂを導管２０ｃおよび２０ｄに備え、上側マニホールド２１は弁２１ａおよび２１ｂを導管２１ｃおよび２１ｄに備え、さらに上側マニホールド２２は弁２２ａおよび２２ｂを導管２２ｃおよび２２ｄに備える。導管２０ｃ、２１ｃおよび２２ｃを硫黄含有ガスの出口導管７に接続すると共に、導管２０ｄ、２１ｄおよび２２ｄを接続導管１０に接続する。
正常操作に際し、硫化水素と化学量論量未満の遊離酸素とを含むガス流を供給物の供給導管４を介すると共に導管１５ｄを介し接触反応器１に供給して多量の硫化水素を除去する。硫化水素含有量の減少した第１精製ガスを導管２０ｄを介して第１接触反応器１から除去すると共に、これを接続導管１０を介し第２接触反応器２へ供給して微量の硫化水素を除去する。追加遊離酸素を別途の供給導管（図示せず）を介して第２接触反応器２へ供給する。全精製ガスを導管１６ｅを介し接触反応器２から除去し、これを精製ガスの出口導管５を介してさらに使用すべく除去する。
【００１１】
同時に接触反応器３における触媒材料を再生し、この目的で熱再生ガスを再生ガスの供給導管６を介すると共に導管１７ｆを介して接触反応器３に供給する。熱ガスの温度は元素硫黄の露点よりも高い。接触反応器３における触媒材料からの硫黄が充填された再生ガスを接触反応器３から導管２２ｃを介して除去すると共に硫黄含有ガスの出口導管７を介し凝縮器８に供給して元素硫黄を凝縮させる。凝縮した硫黄を貯蔵タンク９に貯蔵し、そこから出口導管２５を介して除去することができ、硫黄フリーのガスを貯蔵タンク９から出口導管２６を介して除去する。
この第１期間にて接触反応器１は多量の硫化水素を除去すべく使用され、接触反応器２は微量の硫黄を除去すべく用いられ、さらに接触反応器３における触媒材料は再生される。
【００１２】
第１期間における弁の位置を表２に示す。
変換率が低下し始めるようなレベルまで接触反応器１における触媒材料が充填された際、接触反応器１における触媒材料を再生し、次いで多量の硫化水素の除去を接触反応器２で行うと共に微量の除去を触媒材料が第１期間にて再生された接触反応器３で行う。流れを適切に指向させるには、或る弁を開放させると共に他の弁を閉鎖せねばならず、この第２期間における弁の位置を表２に示す。追加遊離酸素を別途の供給導管（図示せず）を介し第３接触反応器３に供給する。
変換率が低下し始めるようなレベルまで接触反応器２における触媒材料が充填された際、接触反応器２における触媒材料を再生し、多量の硫化水素の除去を接触反応器３で行うと共に微量の除去を触媒材料が第２期間にて再生された接触反応１でて行う。追加遊離酸素を別途の供給導管（図示せず）を介し第１接触反応器１に供給する。流れを適切に指向させるには、或る弁を開放すると共に他の弁を閉鎖せねばならず、この第３期間における各弁の位置を表２に示す。
次いで工程を第１期間と共に継続する。
【００１３】
【表２】
Figure 0003646885
【００１４】
第１期間における以下の仮定例により本発明をさらに例示する。接触反応器１、２および３には、４ｍｍの粒子寸法を有する活性化アルミナ粒子としての６６．８ｍ3 の触媒材料を満たす。
１．０容量％のＨ2 Ｓと１００ｐｐｍｖ（１，０００，０００分の１容量部）のＣＯＳと１容量％のＣＯ2 と０．４８容量％のＯ2 とを含む天然ガスよりなる供給物を６０バールの圧力および１００℃の温度にて導管１５ｄを介し第１接触反応器１中へ移送する。流速は１７０ ０００Ｎｍ3 ／ｈ（１時間当りの標準ｍ3 ）である。反応器内のガス空時速度は２ ５００ｖｏｌ／ｖｏｌ／ｈｒである。この第１接触反応器１にてＨ2 Ｓの９５％が元素硫黄に変換され、これを触媒粒子に吸着させる。触媒粒子は１６．６時間にて７５重量％まで充填され、この時点で第２期を開始する。
反応は発熱性であるため最初の精製ガスは１５０℃の温度にて第１接触反応器１から流出し、このガスを追加量の２５０ｐｐｍｖのＯ2 と一緒に導管２１ｄを介し第２接触反応器２中へ供給すると共に、精製ガスをほぼ同温度にて反応器２から流出させる。精製ガスにおける硫化水素濃度は３０ｐｐｍｖ Ｈ2 Ｓ未満であり、精製ガスにおける元素硫黄の量は３ｐｐｍｖ未満である。
【００１５】
第３接触反応器３における触媒粒子を、６０バールの圧力および４００℃の温度にてガスを第３接触反応器３中に通過させて再生する。２８ １２９ Ｎｍ3 ／ｈのガス流速につき、触媒粒子の再生には約１３時間を要する。再生ガスは、第２接触反応器２から流出する精製ガスの副流とするのが好適である。硫黄の貯蔵タンク９から導管２６を介して流出する硫黄フリーのガスを導管５における精製ガスに添加することができる。
【図面の簡単な説明】
【図１】 本発明による方法を実施するための装置の流れ図。
【符号の説明】
１、２、３ 反応器
４ 供給導管
５ 精製ガスの出口導管
６ 再生ガスの供給導管
７ 硫黄含有ガスの出口導管
８ 凝縮器
９ 硫黄の貯蔵タンク
１０ 接続導管[0001]
[Industrial application fields]
The present invention relates to a method for removing hydrogen sulfide from a gas stream. An example of this type of gas stream is natural gas.
[0002]
[Prior art]
International Patent Application No. 92/02 449 describes a method for removing hydrogen sulfide from a gas stream, wherein the method involves the first catalytic reaction of the gas stream in the presence of free oxygen at a temperature above the dew point of elemental sulfur. Contacting the catalyst material with a reactor to obtain a partially purified gas stream, and the partially purified gas stream with the catalyst material in a second contact reactor at a temperature between the dew point of water and elemental sulfur. It consists in contacting to obtain a purified gas stream.
In this known method, air is supplied to the gas stream upstream of the first catalytic reactor. Free oxygen in the air reacts with hydrogen sulfide in the following reactions:
H 2 S + 1/2 O 2 -----> H 2 O + 1 / x S x
Oxidizes directly to elemental sulfur.
The patent publication is silent on the amount of free oxygen fed to the first catalytic reactor, but this amount is generally stoichiometric or slightly greater than the stoichiometric amount. That is, the ratio between the oxygen and hydrogen sulfide concentrations is 0.5, ie, the stoichiometric ratio or higher. The unit of this ratio is mol / mol or vol / vol at standard pressure and temperature. In this specification, the ratio between the concentrations of oxygen and hydrogen sulfide is referred to as the “oxygen-hydrogen sulfide ratio”.
[0003]
This time, the Applicant has contacted the gas stream with the catalyst material in the first contact reactor so that the elemental sulfur is adsorbed on the catalyst material in the first contact reactor at a temperature between the dew point of water and the dew point of elemental sulfur I suggest that The first catalytic reactor is used to remove a large amount of hydrogen sulfide, and the second catalytic reactor is used to remove a trace amount of hydrogen sulfide from the gas flowing out of the first catalytic reactor.
In the process of the present invention, the first catalytic reactor is used to remove a large amount of hydrogen sulfide from the gas stream, so that the majority of the elemental sulfur produced is adsorbed on the catalytic material in this catalytic reactor. The adsorbed elemental sulfur increases the activity of the catalyst material. However, if the amount of elemental sulfur adsorbed on the catalyst material is higher than a predetermined level, the conversion rate of hydrogen sulfide decreases, which decreases with the amount of sulfur adsorbed on the catalyst material. Therefore, a larger amount of hydrogen sulfide flows out of the first catalytic reactor. In order to reduce hydrogen sulfide leakage, the catalyst material in the first catalytic reactor must be regenerated before the H 2 S conversion falls below a predetermined level. Accordingly, the time between two successive regenerations is determined by the time required to reach the sulfur content in the first catalytic reactor where the H 2 S conversion has fallen below a predetermined level.
[0004]
[Problems to be solved by the invention]
The object of the present invention is to increase the cycle time.
[0005]
[Means for Solving the Problems]
In order to solve the above problems, the method for removing hydrogen sulfide from a gas stream according to the present invention comprises two catalytic reactors in the presence of free oxygen at a temperature ranging from the dew point of water to the dew point of elemental sulfur. To obtain elemental sulfur deposited on the catalyst material and purified gas stream in contact with the catalyst material at a first contact reactor in the presence of less than stoichiometric free oxygen in the first contact reactor. A partially purified gas stream is obtained and this partially purified gas stream is contacted with a catalytic material in the presence of additional free oxygen in a second catalytic reactor to obtain a purified gas quantity.
The present invention is based on the finding that the amount of sulfur in the catalyst material at which the H 2 S-conversion rate decreases depends on the oxygen-hydrogen sulfide ratio. If this ratio is greater than or equal to 0.5, the initial H 2 S-conversion is generally 95-100%, but the sulfur content of the catalyst material where the H 2 S-conversion begins to decrease is less than 40%. . Oxygen - if less than the ratio of hydrogen sulfide 0.5 H 2 S- conversion is less than 95%, sulfur content of catalytic material H 2 S- conversion starts to decrease oxygen - hydrogen sulfide ratio It was found that the H 2 S-conversion rate is about twice the amount of sulfur at which the H 2 S-conversion rate begins to decrease when the value is 0.5 or more. This effect is illustrated in the following example:
Three experiments were performed to determine the H 2 S-conversion rate as a function of the amount of sulfur in the catalyst material. In these experiments, a nitrogen stream saturated with water was used to simulate a methane stream saturated with water. The nitrogen stream further contained 1% by volume H 2 S, 1% by volume CO 2 , 200 ppmv (1,000,000 parts by volume) COS and free oxygen. The amount of free oxygen was selected so that the oxygen-hydrogen sulfide ratios were 0.6, 0.45 and 0.27. The stoichiometric ratio of [O 2 ] to [H 2 S] is 0.5. The catalyst material used was an activated alumina catalyst (A201 from La Roche). The pressure was 10 bar, the temperature was 150 ° C., and the gas space velocity was 2000 vol / vol / hr. Table 1 shows the results of each experiment as the initial H 2 S-conversion rate and sulfur content of the catalyst as the conversion rate begins to drop as a function of the oxygen-hydrogen sulfide ratio. The initial H 2 S conversion is 1- [H 2 S] out / [H 2 S] in (where [H 2 S] in is the concentration of hydrogen sulfide in the gas stream flowing into the catalytic reactor, H 2 S] out is the concentration of hydrogen sulfide in the gas stream leaving the catalytic reactor. The amount of sulfur in the catalyst is expressed as kg of sulfur per kg of catalyst.
[0007]
[Table 1]
Figure 0003646885
[0008]
Suitably the oxygen-hydrogen sulfide ratio of the process according to the invention in the gas stream flowing into the first catalytic reactor is in the range of 0.40 to 0.49, more preferably in the range of 0.45 to 0.49. .
The second catalytic reactor is used to remove traces of hydrogen sulfide, and a partially purified gas stream for this purpose is contacted with the catalytic material in the presence of additional free oxygen in the second catalytic reactor. The amount of additional free oxygen is selected such that the total amount of oxygen, with the initial amount of hydrogen sulfide present in the gas stream, is equal to or greater than the stoichiometric amount.
[0009]
The invention will now be described in more detail by way of example with reference to the accompanying drawings which show an apparatus for carrying out the method according to the invention.
The apparatus comprises three reactors containing the catalyst materials indicated by reference numerals 1, 2 and 3, a feed supply conduit 4, a purified gas outlet conduit 5, a regeneration gas supply conduit 6, and a sulfur-containing gas. The outlet conduit 7, the condenser 8, the sulfur storage tank 9, and the connecting conduit 10.
Each catalytic reactor 1, 2 and 3 has a lower manifold, indicated by reference numerals 15, 16 and 17. Lower manifold 15 includes valves 15a, 15b and 15c in conduits 15d, 15e and 15f, lower manifold 16 includes valves 16a, 16b and 16c in conduits 16d, 16e and 16f, and lower manifold 17 includes valve 17a. 17b and 17c are provided in the conduits 17d, 17e and 17f. Conduits 15d, 16d and 17d are connected to the feed supply conduit 4, conduits 15e, 16e and 17e are connected to the purified gas outlet conduit 5, and conduits 15f, 16f and 17f are connected to the regeneration gas supply conduit 6. Is done.
[0010]
Furthermore, each catalytic reactor 1, 2 and 3 also comprises an upper manifold, indicated by reference numerals 20, 21 and 22. Upper manifold 20 includes valves 20a and 20b in conduits 20c and 20d, upper manifold 21 includes valves 21a and 21b in conduits 21c and 21d, and upper manifold 22 includes valves 22a and 22b in conduits 22c and 22d. The conduits 20c, 21c and 22c are connected to the sulfur containing gas outlet conduit 7 and the conduits 20d, 21d and 22d are connected to the connecting conduit 10.
During normal operation, a gas stream containing hydrogen sulfide and less than stoichiometric free oxygen is supplied to the contact reactor 1 through the feed supply conduit 4 and through the conduit 15d to remove large amounts of hydrogen sulfide. The first purified gas having a reduced hydrogen sulfide content is removed from the first catalytic reactor 1 via the conduit 20d and supplied to the second catalytic reactor 2 via the connecting conduit 10 to produce a trace amount of hydrogen sulfide. Remove. Additional free oxygen is fed to the second catalytic reactor 2 via a separate feed conduit (not shown). All purified gas is removed from the contact reactor 2 via conduit 16e and removed via the purified gas outlet conduit 5 for further use.
[0011]
At the same time, the catalyst material in the catalytic reactor 3 is regenerated, and for this purpose, the heat regeneration gas is supplied to the catalytic reactor 3 via the regeneration gas supply conduit 6 and via the conduit 17f. The temperature of the hot gas is higher than the dew point of elemental sulfur. The regeneration gas filled with sulfur from the catalyst material in the catalytic reactor 3 is removed from the catalytic reactor 3 through a conduit 22c and supplied to a condenser 8 through a sulfur-containing gas outlet conduit 7 to condense elemental sulfur. Let Condensed sulfur can be stored in storage tank 9 and removed therefrom through outlet conduit 25 and sulfur-free gas removed from storage tank 9 through outlet conduit 26.
In this first period, the catalytic reactor 1 is used to remove a large amount of hydrogen sulfide, the catalytic reactor 2 is used to remove a trace amount of sulfur, and the catalyst material in the catalytic reactor 3 is regenerated.
[0012]
Table 2 shows the position of the valve in the first period.
When the catalytic material in the catalytic reactor 1 is charged to such a level that the conversion rate begins to decrease, the catalytic material in the catalytic reactor 1 is regenerated, and then a large amount of hydrogen sulfide is removed in the catalytic reactor 2 and a trace amount is removed. Is removed in the catalytic reactor 3 in which the catalyst material is regenerated in the first period. In order to properly direct the flow, one valve must be opened and the other valve closed, and the position of the valve in this second period is shown in Table 2. Additional free oxygen is fed to the third catalytic reactor 3 via a separate feed conduit (not shown).
When the catalytic material in the catalytic reactor 2 is charged to such a level that the conversion rate starts to decrease, the catalytic material in the catalytic reactor 2 is regenerated, and a large amount of hydrogen sulfide is removed by the catalytic reactor 3 and a small amount of hydrogen is removed. Removal takes place in catalytic reaction 1 in which the catalyst material is regenerated in the second period. Additional free oxygen is fed to the first catalytic reactor 1 via a separate feed conduit (not shown). To properly direct the flow, certain valves must be opened and other valves closed, and the position of each valve in this third period is shown in Table 2.
The process then continues with the first period.
[0013]
[Table 2]
Figure 0003646885
[0014]
The invention is further illustrated by the following hypothetical example in the first period. Catalytic reactors 1, 2 and 3 are filled with 66.8 m 3 of catalytic material as activated alumina particles having a particle size of 4 mm.
A feed consisting of natural gas containing 1.0% by volume H 2 S, 100 ppmv (parts per 1,000,000 parts) COS, 1% by volume CO 2 and 0.48% by volume O 2 . Is transferred into the first catalytic reactor 1 via line 15d at a pressure of 60 bar and a temperature of 100 ° C. The flow rate is 170 000 Nm 3 / h (standard m 3 per hour). The gas space-time velocity in the reactor is 2500 vol / vol / hr. In the first contact reactor 1, 95% of H 2 S is converted to elemental sulfur, which is adsorbed on the catalyst particles. The catalyst particles are loaded to 75% by weight in 16.6 hours, at which point the second phase begins.
Since the reaction is exothermic, the first purified gas flows out of the first catalytic reactor 1 at a temperature of 150 ° C., and this gas is combined with an additional amount of 250 ppmv O 2 through the conduit 21d into the second catalytic reactor. The purified gas is discharged from the reactor 2 at approximately the same temperature. The hydrogen sulfide concentration in the purified gas is less than 30 ppmv H 2 S, and the amount of elemental sulfur in the purified gas is less than 3 ppmv.
[0015]
The catalyst particles in the third catalytic reactor 3 are regenerated by passing gas through the third catalytic reactor 3 at a pressure of 60 bar and a temperature of 400 ° C. For a gas flow rate of 28 129 Nm 3 / h, regeneration of the catalyst particles takes about 13 hours. The regeneration gas is preferably a side stream of the purified gas flowing out from the second catalytic reactor 2. Sulfur-free gas exiting from the sulfur storage tank 9 via conduit 26 can be added to the purified gas in conduit 5.
[Brief description of the drawings]
1 is a flow chart of an apparatus for carrying out the method according to the invention.
[Explanation of symbols]
1, 2, 3 Reactor 4 Supply conduit 5 Purified gas outlet conduit 6 Regenerative gas supply conduit 7 Sulfur-containing gas outlet conduit 8 Condenser 9 Sulfur storage tank 10 Connection conduit

Claims (2)

ガス流から硫化水素を除去するに際し、ガス流を遊離酸素の存在下に水の露点〜元素硫黄の露点の範囲の温度にて２個の接触反応器で触媒材料と接触させて触媒材料上に沈着する元素硫黄と精製ガス流とを得、ガス流を第１接触反応器にて化学量論未満の量の遊離酸素の存在下に触媒材料と接触させて部分精製されたガス流を得、この部分精製されたガス流を第２接触反応器で追加遊離酸素の存在下に触媒材料と接触させて精製ガス流を得ることを特徴とするガス流からの硫化水素の除去方法。In removing hydrogen sulfide from a gas stream, the gas stream is contacted with the catalyst material in two contact reactors in the presence of free oxygen at a temperature ranging from the dew point of water to the dew point of elemental sulfur. Obtaining elemental sulfur to be deposited and a purified gas stream, contacting the gas stream with a catalytic material in the presence of a sub-stoichiometric amount of free oxygen in a first catalytic reactor to obtain a partially purified gas stream; A method for removing hydrogen sulfide from a gas stream, wherein the partially purified gas stream is contacted with a catalytic material in the presence of additional free oxygen in a second catalytic reactor to obtain a purified gas stream. ガス流を第１接触反応器にて酸素−硫化水素の比が０．４０〜０．４９の範囲となるような量の遊離酸素の存在下に触媒材料と接触させる請求項１に記載の方法。The process of claim 1, wherein the gas stream is contacted with the catalyst material in the presence of free oxygen in an amount such that the oxygen-hydrogen sulfide ratio is in the range of 0.40 to 0.49 in the first catalytic reactor. .
JP33756594A 1994-12-28 1994-12-28 Removal of hydrogen sulfide from gas streams Expired - Fee Related JP3646885B2 (en)

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