JPH08290904A - Treatment of tail gas in sulfur recovery unit - Google Patents
Treatment of tail gas in sulfur recovery unitInfo
- Publication number
- JPH08290904A JPH08290904A JP7114026A JP11402695A JPH08290904A JP H08290904 A JPH08290904 A JP H08290904A JP 7114026 A JP7114026 A JP 7114026A JP 11402695 A JP11402695 A JP 11402695A JP H08290904 A JPH08290904 A JP H08290904A
- Authority
- JP
- Japan
- Prior art keywords
- tail gas
- gas
- hydrogen sulfide
- sulfur
- sulfur recovery
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Abstract
Description
【０００１】[0001]
【産業上の利用分野】本発明は硫黄回収装置におけるテ
ールガスの処理方法に関する。FIELD OF THE INVENTION The present invention relates to a method for treating tail gas in a sulfur recovery system.
【０００２】[0002]
【従来の技術】硫黄回収装置は、硫化水素を含有する比
較的大量のガス、例えば天然ガス，石油製油所副生ガ
ス，コークス炉ガス等を吸収液再生式の吸収装置で処理
して、吸収液を再生して得られる硫化水素を原料にし
て、次記のいわゆるクラウス反応により、元素状硫黄を
回収する装置であり、特に石油製油所において広く利用
されている。 Ｈ2 Ｓ＋3/2 Ｏ2 → ＳＯ2 ＋Ｈ2 Ｏ ２Ｈ2 Ｓ＋ＳＯ2 → ３Ｓ＋２Ｈ2 Ｏ 上記の反応式からも明らかなように、原料硫化水素の３
分の１を反応炉で空気で酸化して二酸化硫黄となし、次
いでこの二酸化硫黄と残りの硫化水素をアルミナ系触媒
充填のコンバータで反応させて、元素状硫黄に転換し回
収している。2. Description of the Related Art A sulfur recovery apparatus treats a relatively large amount of gas containing hydrogen sulfide, for example, natural gas, petroleum refinery by-product gas, coke oven gas, etc., with an absorption liquid regeneration type absorption apparatus and absorbs it. This is a device for recovering elemental sulfur by the so-called Claus reaction described below using hydrogen sulfide obtained by regenerating the liquid as a raw material, and is widely used particularly in petroleum refineries. H 2 S + 3/2 O 2 → SO 2 + H 2 O 2H 2 S + SO 2 → 3S + 2H 2 O As is clear from the above reaction formula, 3
One part is oxidized with air in a reaction furnace to form sulfur dioxide, and then this sulfur dioxide and the remaining hydrogen sulfide are reacted with a converter filled with an alumina-based catalyst to be converted into elemental sulfur and recovered.
【０００３】しかしながら反応の平衡上、硫黄回収装置
を出る排出ガス（以下、テールガスという）には、未反
応の硫化水素，二酸化硫黄及びＣＳ2 ，ＣＯＳ等有機硫
黄化合物が含まれており、元素状硫黄の回収率はコンバ
ータの段数を多くすれば高くなるが、それでも３段のコ
ンバータを用いても９７〜９８％程度であり、すなわち
原料硫化水素の２〜３％に相当する硫黄化合物が、テー
ルガス中に残存して、大気放出されることになる。However, due to reaction equilibrium, the exhaust gas (hereinafter referred to as tail gas) exiting the sulfur recovery device contains unreacted hydrogen sulfide, sulfur dioxide and organic sulfur compounds such as CS 2 and COS. Although the recovery rate of sulfur increases as the number of stages of the converter increases, it is still about 97 to 98% even when a three-stage converter is used, that is, the sulfur compound corresponding to 2 to 3% of the raw hydrogen sulfide is tail gas. It remains inside and is released into the atmosphere.
【０００４】現在迄、このテールガス中の硫黄化合物を
処理する方法として、次の二つの方法が実施されてい
る。第１の方法は、テールガスの全量を助燃剤を用いて
燃焼炉で燃焼して、硫黄化合物を全て二酸化硫黄に酸化
し、次いで公知の排煙脱硫装置に通して、この二酸化硫
黄をアルカリ性吸収液で吸収除去する方法である。この
際、排煙脱硫方法としては、通常の水マグ法，芒硝法等
が用いられるが、いずれも水酸化マグネシウム，苛性ソ
ーダ等の薬品代が嵩むこと、硫酸マグネシウム，硫酸ナ
トリウム等を含む相当量の排水が発生する等の問題があ
る。To date, the following two methods have been carried out as a method of treating the sulfur compound in the tail gas. In the first method, all of the tail gas is burned in a combustion furnace using a combustion improver to oxidize all sulfur compounds to sulfur dioxide, and then the sulfur gas is passed through a known flue gas desulfurization device to convert the sulfur dioxide into an alkaline absorption liquid. It is a method of absorbing and removing with. At this time, as a flue gas desulfurization method, an ordinary water-magnification method, a sodium sulfate method, etc. are used. There are problems such as drainage.
【０００５】第２の方法は、英国の石油会社であるシェ
ル社が開発し、特公昭５７−１６８４６号で開示された
方法（SCOT法と呼ばれている) である。この方法の概要
は次の通りである。すなわち、テールガスに水素ガスを
添加して、所定の温度下で水素添加触媒を充填した反応
器を通して、テールガス中の硫黄化合物を全て硫化水素
に転換する。次いでテールガス処理専用に設けられる吸
収液再生式のガス吸収装置に通して、前記の転換した硫
化水素をアミン系の吸収液にて選択吸収してから、吸収
液を再生塔にてスチームストリッピングして、駆出され
る硫化水素をクラウス式硫黄回収装置に循環供給して処
理する方法である。The second method is a method developed by the British oil company Shell Company and disclosed in Japanese Patent Publication No. 57-16846 (called the SCOT method). The outline of this method is as follows. That is, hydrogen gas is added to the tail gas, and all the sulfur compounds in the tail gas are converted to hydrogen sulfide through a reactor filled with a hydrogenation catalyst at a predetermined temperature. Then, it is passed through an absorption liquid regeneration type gas absorption device provided exclusively for tail gas treatment, and after the converted hydrogen sulfide is selectively absorbed by an amine-based absorption liquid, the absorption liquid is steam stripped in a regeneration tower. Then, the hydrogen sulfide ejected is circulated and supplied to the Claus sulfur recovery device for processing.
【０００６】この方法では、ガス吸収装置でテールガス
中の転換した硫化水素の全てを吸収できないため、焼却
炉を設けてガス吸収装置を出るテールガスをこの焼却炉
に導入し、助燃剤を用いてテールガスに残存している硫
化水素を二酸化硫黄に酸化して煙突を介して大気放出し
なければならないという問題がある。また、ガス吸収装
置は、吸収塔，再生塔，吸収液循環ポンプ，吸収液再生
リボイラー等から構成される複雑な設備であり、さらに
は吸収液の再生に必要な熱量も多量であるため、設備費
及び運転費の両面で経済的負担が大きいという問題があ
る。In this method, since all of the converted hydrogen sulfide in the tail gas cannot be absorbed by the gas absorption device, an incinerator is provided, and the tail gas exiting the gas absorption device is introduced into this incinerator, and the tail gas is added using the combustion improver. There is a problem that the remaining hydrogen sulfide must be oxidized to sulfur dioxide and released to the atmosphere through the chimney. In addition, the gas absorption device is a complex facility including an absorption tower, a regeneration tower, an absorption liquid circulation pump, an absorption liquid regeneration reboiler, and the like, and since the amount of heat required to regenerate the absorption liquid is large, There is a problem that the financial burden is large in terms of both operating and operating costs.
【０００７】[0007]
【発明が解決しようとする課題】本発明は、以上の従来
技術の問題点に鑑みてなされたものであって、装置から
出る排ガス，排水等の二次公害問題の全くないクローズ
ドシステムであって、設備費が少なく、なお且つ、薬品
代等の運転経費の負担の少ない硫黄回収装置におけるテ
ールガスの処理方法を提供することを目的とする。SUMMARY OF THE INVENTION The present invention has been made in view of the above problems of the prior art, and is a closed system having no secondary pollution problem such as exhaust gas and drainage from the apparatus. An object of the present invention is to provide a method for treating tail gas in a sulfur recovery apparatus that has low equipment costs and low operating costs such as chemical costs.
【０００８】[0008]
【課題を解決するための手段】本発明の要旨とするとこ
ろは、硫化水素を含有するガスを吸収液再生式吸収装置
で処理し、吸収液を再生して得られる硫化水素を原料に
してクラウス反応により元素状硫黄を回収する硫黄回収
装置において、前記硫黄回収装置を排出するテールガス
を所定温度に昇温して水素または水素含有ガスを注入し
た後に、水素添加触媒に通して、前記テールガス中の硫
黄化合物を硫化水素に転換し、所定温度に冷却してから
前記吸収液再生式吸収装置に循環供給して処理すること
を特徴とする硫黄回収装置におけるテールガスの処理方
法にある。SUMMARY OF THE INVENTION The gist of the present invention is to use a hydrogen sulfide obtained by treating a gas containing hydrogen sulfide with an absorption liquid regeneration type absorption device and regenerating the absorption liquid as a raw material. In a sulfur recovery apparatus for recovering elemental sulfur by a reaction, the tail gas discharged from the sulfur recovery apparatus is heated to a predetermined temperature and hydrogen or a hydrogen-containing gas is injected, and then passed through a hydrogenation catalyst, A method for treating tail gas in a sulfur recovery apparatus is characterized in that a sulfur compound is converted to hydrogen sulfide, cooled to a predetermined temperature, and then circulated and supplied to the absorption liquid regenerating absorption apparatus for processing.
【０００９】[0009]
【作用】硫黄回収装置から排出するテールガスに水素ま
たは水素含有ガスを注入して、ニッケルーモリブデン系
等の水添触媒上で、水添反応に好適な温度；３００〜４
００℃でテールガス中の硫黄化合物を水素化して、硫化
水素に転換する。このあと、転換した硫化水素を含むテ
ールガスを、硫黄回収装置に原料の硫化水素を供給する
吸収液再生式吸収装置に循環供給して、硫化水素を選択
吸収し、再生塔で吸収液から駆出される硫化水素は硫黄
回収装置に送られて、元素状硫黄として回収される。以
上から分かるように、テールガス専用の吸収液再生式吸
収装置が不要であり、且つ排水、排ガス等の二次公害の
無いクローズドシステムからなる処理方法であることが
分かる。Operation: Hydrogen or a hydrogen-containing gas is injected into the tail gas discharged from the sulfur recovery unit, and the temperature suitable for the hydrogenation reaction is 300 to 4 on a hydrogenation catalyst such as a nickel-molybdenum system.
The sulfur compounds in the tail gas are hydrogenated at 00 ° C and converted to hydrogen sulfide. After that, the tail gas containing the converted hydrogen sulfide is circulated and supplied to the absorption liquid regeneration absorption device that supplies the raw material hydrogen sulfide to the sulfur recovery device, selectively absorbing hydrogen sulfide, and ejected from the absorption liquid in the regeneration tower. The generated hydrogen sulfide is sent to a sulfur recovery device and recovered as elemental sulfur. As can be seen from the above, it is understood that the treatment method is a closed system that does not require an absorption liquid regeneration type absorption device dedicated to tail gas and does not cause secondary pollution of waste water, exhaust gas and the like.
【００１０】[0010]
【実施例】以下、本発明の実施例について説明する。図
１は、本発明の実施例の系統図である。硫化水素を含有
するガス、例えば石油製油所における各精製工程におい
て副生するガス、あるいは製鉄所のコークス製造工場に
おいて副生するコークス炉ガス等は、多量の硫化水素を
含んでおり、またガス量も多量であるため、吸収液再生
式の吸収装置を設け、硫化水素を選択的に吸収するアミ
ン系あるいはアンモニア等のアルカリ性の水溶液を吸収
液として用い、吸収塔にて気液接触させて吸収除去して
いる。そして吸収塔を出る硫化水素リッチの吸収液は、
再生塔に導入してスチームストリッピングされ、塔頂か
ら駆出される硫化水素は硫黄回収装置に供給されて、反
応炉および２〜３段のアルミナ系触媒を充填するコンバ
ータにて、前記のクラウス反応により、元素状硫黄に転
換され、各段コンバータの下流に設けられるコンデンサ
にて凝縮して回収される。Embodiments of the present invention will be described below. FIG. 1 is a system diagram of an embodiment of the present invention. A gas containing hydrogen sulfide, for example, a gas that is a byproduct of each refining process in a petroleum refinery, or a coke oven gas that is a byproduct of a coke manufacturing plant in an iron refinery contains a large amount of hydrogen sulfide, and the amount of gas is also large. Since it is a large amount, an absorption liquid regeneration type absorption device is installed, and an amine-based or alkaline aqueous solution such as ammonia that selectively absorbs hydrogen sulfide is used as the absorption liquid, and it is absorbed and removed by contacting it with gas-liquid in the absorption tower. are doing. And the hydrogen sulfide-rich absorbent that exits the absorption tower is
The hydrogen sulfide introduced into the regeneration tower, steam stripped, and ejected from the top of the tower is supplied to the sulfur recovery device, and is fed into the reactor and a converter that is filled with 2 to 3 stages of alumina-based catalyst. By this, it is converted into elemental sulfur and is condensed and recovered by a condenser provided downstream of each stage converter.
【００１１】硫黄回収装置の最終段のコンバータ及びコ
ンデンサを出るテールガス中には、前記のように回収率
に応じて２〜３％の硫黄化合物が残存している。これら
の硫黄化合物を全て硫化水素に転換するため、テールガ
スを水素添加還元反応に好適な温度：３００〜４００℃
に昇温する。昇温方法は、直火式の加熱炉による間接昇
温、あるいは昇温炉での助燃剤を燃焼する直接昇温など
が適宜用いられる。昇温後のテールガスは、ニッケル−
モリブデン系あるいはコバルト−モリブデン系等の通常
の水素添加触媒が充填された反応器に供給される。空間
速度としては５００〜１５００（１／Ｈｒ）の範囲であ
り、テールガス中の酸化硫黄，元素硫黄，二硫化炭素等
の硫黄化合物は、注入された水素ガスと反応して、硫化
水素に転換される。In the tail gas exiting the converter and the condenser at the final stage of the sulfur recovery apparatus, 2-3% of sulfur compounds remain depending on the recovery rate as described above. Since all of these sulfur compounds are converted to hydrogen sulfide, the tail gas is suitable for hydrogenation reduction reaction at a temperature of 300 to 400 ° C.
The temperature rises to. As the temperature raising method, an indirect temperature raising by a direct-fired heating furnace, a direct temperature raising by burning the combustion improver in the temperature raising furnace, or the like is appropriately used. The tail gas after heating is nickel-
It is supplied to a reactor filled with a usual hydrogenation catalyst such as molybdenum type or cobalt-molybdenum type. The space velocity is in the range of 500 to 1500 (1 / Hr), and sulfur compounds such as sulfur oxide, elemental sulfur and carbon disulfide in the tail gas react with the injected hydrogen gas and are converted into hydrogen sulfide. It
【００１２】反応器を出る硫黄化合物が硫化水素に転換
された高温のテールガスは、熱回収をするため廃熱ボイ
ラに通した後に、さらに冷却水による冷却器を通してほ
ぼ常温近くまで冷却される。そして転換した硫化水素を
吸収除去するため、前記の製油所副生ガスの硫化水素吸
収装置に循環供給される。この循環の際、処理系統全体
の圧力バランスの関係で、テールガスの昇圧が必要の場
合は、ブローワあるいは圧縮機等のガス循環機を設けて
適宜昇圧してから、硫化水素吸収装置に供給する。The high-temperature tail gas in which the sulfur compounds leaving the reactor have been converted into hydrogen sulfide is passed through a waste heat boiler for heat recovery, and is then cooled to near normal temperature through a cooler with cooling water. Then, in order to absorb and remove the converted hydrogen sulfide, it is circulated and supplied to the hydrogen sulfide absorbing device for the by-product gas of the refinery. During this circulation, if the pressure of the tail gas needs to be increased due to the pressure balance of the entire processing system, a gas circulator such as a blower or a compressor is provided to appropriately increase the pressure, and then the tail gas is supplied to the hydrogen sulfide absorber.
【００１３】硫化水素吸収装置においては、循環して供
給されるテールガスは、製油所副生ガスと合流して、そ
れぞれガス中の硫化水素は、吸収塔においてアミン系あ
るいはアンモニア等のアルカリ水溶液により吸収され
る。吸収塔を出る硫化水素リッチの吸収液は、再生塔に
導入されてスチームストリッピングされ、塔頂から駆出
される硫化水素は、硫黄回収装置に供給されて、前記の
クラウス反応により元素状硫黄として回収される。In the hydrogen sulfide absorber, the tail gas circulated and supplied merges with the refinery by-product gas, and the hydrogen sulfide in each gas is absorbed by an amine system or an alkaline aqueous solution such as ammonia in the absorption tower. To be done. The hydrogen sulfide-rich absorption liquid leaving the absorption tower is introduced into the regeneration tower and steam stripped, and the hydrogen sulfide ejected from the top of the tower is supplied to the sulfur recovery device, and as elemental sulfur by the Claus reaction described above. Be recovered.
【００１４】[0014]
【発明の効果】以上の構成と作用を有する本発明によれ
ば、次のような効果が得られるので、本発明は産業上極
めて有益である。 (1) 硫黄回収装置を出るテールガスは、クローズドタイ
プのシステムで処理されるため、排ガス, 排水発生等の
二次公害の問題がない。 (2) 排煙脱硫装置などで必要な、アルカリ薬品代が不要
なため、運転経費が安くなる。 (3) テールガス専用の硫化水素吸収装置の設置が不要に
なるため、設備費の負担が非常に少なくなる。According to the present invention having the above-mentioned structure and operation, the following effects can be obtained, so that the present invention is extremely useful industrially. (1) The tail gas that exits the sulfur recovery system is treated by a closed type system, so there is no problem of secondary pollution such as generation of exhaust gas and waste water. (2) The operating costs are reduced because there is no need for alkaline chemicals required for flue gas desulfurization equipment. (3) Since the installation of a hydrogen sulfide absorber dedicated to tail gas is not required, the burden of equipment costs is greatly reduced.
【図１】本発明の処理方法の実施例の系統図。FIG. 1 is a system diagram of an embodiment of a treatment method of the present invention.
Claims (1)
収装置で処理し、吸収液を再生して得られる硫化水素を
原料にしてクラウス反応により元素状硫黄を回収する硫
黄回収装置において、前記硫黄回収装置を排出するテー
ルガスを所定温度に昇温して水素または水素含有ガスを
注入した後に、水素添加触媒に通して、前記テールガス
中の硫黄化合物を硫化水素に転換し、所定温度に冷却し
てから前記吸収液再生式吸収装置に循環供給して処理す
ることを特徴とする硫黄回収装置におけるテールガスの
処理方法。1. A sulfur recovery device for recovering elemental sulfur by Claus reaction using hydrogen sulfide obtained by regenerating an absorption liquid by treating a gas containing hydrogen sulfide with an absorption liquid regeneration type absorption device, After the tail gas discharged from the sulfur recovery device is heated to a predetermined temperature and hydrogen or a hydrogen-containing gas is injected, it is passed through a hydrogenation catalyst to convert the sulfur compound in the tail gas into hydrogen sulfide and cooled to a predetermined temperature. Then, the tail gas processing method in the sulfur recovery apparatus is characterized in that the absorbent is recirculated and supplied to the absorbent regenerator for processing.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP7114026A JPH08290904A (en) | 1995-04-17 | 1995-04-17 | Treatment of tail gas in sulfur recovery unit |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP7114026A JPH08290904A (en) | 1995-04-17 | 1995-04-17 | Treatment of tail gas in sulfur recovery unit |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH08290904A true JPH08290904A (en) | 1996-11-05 |
Family
ID=14627189
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP7114026A Pending JPH08290904A (en) | 1995-04-17 | 1995-04-17 | Treatment of tail gas in sulfur recovery unit |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH08290904A (en) |
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2002032810A1 (en) * | 2000-10-18 | 2002-04-25 | Jgc Corporation | Method and apparatus for removing sulfur compound in gas containing hydrogen sulfide, mercaptan, carbon dioxide and aromatic hydrocarbon |
| WO2007065884A1 (en) * | 2005-12-07 | 2007-06-14 | Shell Internationale Research Maatschappij B.V. | Process for the removal of sulphur compounds and carbon dioxide from a gas stream |
| WO2007065765A1 (en) * | 2005-11-04 | 2007-06-14 | Shell Internationale Research Maatschappij B.V. | Process for producing a purified gas stream |
| WO2010060975A1 (en) * | 2008-11-28 | 2010-06-03 | Shell Internationale Research Maatschappij B.V. | Process for producing purified natural gas |
| JP2010536573A (en) * | 2007-08-30 | 2010-12-02 | シエル・インターナシヨネイル・リサーチ・マーチヤツピイ・ベー・ウイ | Method for removing hydrogen sulfide and carbon dioxide from an acid gas stream |
| CN102631827A (en) * | 2012-04-11 | 2012-08-15 | 山东三维石化工程股份有限公司 | Zero-emission sulfur recovery technology combined with low-temperature methanol washing acid gas treatment |
| US8524189B2 (en) | 2008-11-28 | 2013-09-03 | Shell Oil Company | Process for the selective oxidation of hydrogen sulphide |
| CN106215698A (en) * | 2016-07-21 | 2016-12-14 | 金川集团股份有限公司 | A kind of spent acid processes absorption plant and the method thereof of hydrogen sulfide-containing tail gas |
-
1995
- 1995-04-17 JP JP7114026A patent/JPH08290904A/en active Pending
Cited By (16)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2002032810A1 (en) * | 2000-10-18 | 2002-04-25 | Jgc Corporation | Method and apparatus for removing sulfur compound in gas containing hydrogen sulfide, mercaptan, carbon dioxide and aromatic hydrocarbon |
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