JPH0218129B2 - - Google Patents
Info
- Publication number
- JPH0218129B2 JPH0218129B2 JP57034981A JP3498182A JPH0218129B2 JP H0218129 B2 JPH0218129 B2 JP H0218129B2 JP 57034981 A JP57034981 A JP 57034981A JP 3498182 A JP3498182 A JP 3498182A JP H0218129 B2 JPH0218129 B2 JP H0218129B2
- Authority
- JP
- Japan
- Prior art keywords
- sulfur
- pipe
- desulfurization
- liquid
- gas
- 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.)
- Expired - Lifetime
Links
- 238000000034 method Methods 0.000 claims description 19
- 239000007789 gas Substances 0.000 claims description 12
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 claims description 6
- 241000894006 Bacteria Species 0.000 claims description 5
- 229910000037 hydrogen sulfide Inorganic materials 0.000 claims description 5
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 3
- 238000006555 catalytic reaction Methods 0.000 claims description 3
- 229910052760 oxygen Inorganic materials 0.000 claims description 3
- 239000001301 oxygen Substances 0.000 claims description 3
- 230000001172 regenerating effect Effects 0.000 claims description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 17
- 239000007788 liquid Substances 0.000 description 17
- 229910052717 sulfur Inorganic materials 0.000 description 17
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 16
- 239000011593 sulfur Substances 0.000 description 16
- 238000006477 desulfuration reaction Methods 0.000 description 13
- 230000023556 desulfurization Effects 0.000 description 13
- 230000003647 oxidation Effects 0.000 description 11
- 238000007254 oxidation reaction Methods 0.000 description 11
- 239000007787 solid Substances 0.000 description 8
- 239000010802 sludge Substances 0.000 description 7
- 239000000706 filtrate Substances 0.000 description 5
- 238000000926 separation method Methods 0.000 description 5
- 239000002699 waste material Substances 0.000 description 5
- 238000004519 manufacturing process Methods 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 241000605222 Acidithiobacillus ferrooxidans Species 0.000 description 3
- 239000006228 supernatant Substances 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 238000005273 aeration Methods 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 230000001580 bacterial effect Effects 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 235000015097 nutrients Nutrition 0.000 description 2
- 230000008929 regeneration Effects 0.000 description 2
- 238000011069 regeneration method Methods 0.000 description 2
- 150000003463 sulfur Chemical class 0.000 description 2
- 229920000742 Cotton Polymers 0.000 description 1
- 239000005909 Kieselgur Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 238000005276 aerator Methods 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 239000010425 asbestos Substances 0.000 description 1
- 239000003610 charcoal Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 230000018044 dehydration Effects 0.000 description 1
- 238000006297 dehydration reaction Methods 0.000 description 1
- 230000003009 desulfurizing effect Effects 0.000 description 1
- 230000029087 digestion Effects 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 229910000358 iron sulfate Inorganic materials 0.000 description 1
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 description 1
- RUTXIHLAWFEWGM-UHFFFAOYSA-H iron(3+) sulfate Chemical compound [Fe+3].[Fe+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O RUTXIHLAWFEWGM-UHFFFAOYSA-H 0.000 description 1
- 229910000360 iron(III) sulfate Inorganic materials 0.000 description 1
- 238000005065 mining Methods 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 229910052895 riebeckite Inorganic materials 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 239000002893 slag Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
Landscapes
- Preparation Of Compounds By Using Micro-Organisms (AREA)
- Treating Waste Gases (AREA)
Description
【発明の詳細な説明】
本発明は、バイオガス及び各種鉱工業にて発生
するガス中の硫化水素の除去方法に関する。DETAILED DESCRIPTION OF THE INVENTION The present invention relates to a method for removing hydrogen sulfide from biogas and gases generated in various mining industries.
硫化水素（H2S）は、悪臭が強く、燃焼によつ
てSOxとなり、又パルプ廃液等の嫌気性消化を阻
害する等の問題があるため、従来よりガス中の
H2Sの除去方法が種々検討されてきた。 Hydrogen sulfide (H 2 S) has a strong odor, turns into SOx when burned, and has problems such as inhibiting the anaerobic digestion of pulp waste liquid, etc., so it has traditionally been used in gases.
Various methods for removing H 2 S have been studied.
従来、このH2Sの除去方法として固形のFe
（OH）3等の脱硫剤を用いる乾式法と水又はアル
カリ水溶液による湿式法が実施されてきた。 Conventionally, solid Fe was used as a method for removing H 2 S.
A dry method using a desulfurizing agent such as (OH) 3 and a wet method using water or an aqueous alkali solution have been carried out.
しかしながら、前記乾式法は、大量のガス処理
がH2S濃度の高いガスには不適であり、運転管理
が困難で安全面にも問題がある。 However, the dry method is not suitable for processing a large amount of gas with a high concentration of H 2 S, is difficult to manage, and has safety problems.
一方、湿式法は乾式法に比べ大量のガス処理が
可能であり、水又はアルカリ水溶液に一旦吸収し
たH2Sをイオウまで酸化する酸化法と温度圧力条
件を変えてストリツピングする平衡法が提案され
ている。しかしながら、特に前者は副反応が起こ
りやすく、後者はH2Sの除去効率が十分ではなく
通常H2Sの80％の回収が限度であり、両者ともに
多量の悪臭廃水が発生するため更にこれを処理し
なければならず、イオウの回収に手間がかかると
いう欠点があつた。 On the other hand, the wet method is capable of processing a large amount of gas compared to the dry method, and two methods have been proposed: an oxidation method that oxidizes H 2 S once absorbed in water or an alkaline aqueous solution to sulfur, and an equilibrium method that strips by changing temperature and pressure conditions. ing. However, the former is particularly prone to side reactions, and the latter has insufficient H 2 S removal efficiency and is usually limited to recovery of 80% of H 2 S. Both generate a large amount of foul-smelling wastewater, so this is even more difficult. The drawback was that it had to be treated and it took time and effort to recover the sulfur.
又は、従来いずれの方法もランニングコストが
高く経済的にも不利であつた。 Moreover, all conventional methods have high running costs and are economically disadvantageous.
本発明の目的は、前記欠点を解決したH2Sの除
去方法、即ち、脱硫効率に優れ大量のガス処理が
可能でイオウの回収も容易であり、大がかりな設
備を必要とせず、経済的に有利なH2Sの除去方法
を提供することにあり、本発明者らは鋭意検討を
重ねた結果、ガス中のH2Sを硫酸第二鉄〔Fe2
（SO4）3〕水溶液に接触反応させることによつて、
非常に優れたH2Sの除去効率が得られH2Sの除去
と固形イオウの生成が同時に行われることを見い
出し、更にFe2（SO4）3水溶液として、鉄酸化バク
テリア及び酸素の存在下で前記接触反応により生
成するFeSO4及びH2SO4によつて再生せしめたも
のを使用することによつて本発明の目的が全て達
成され本発明を完成するに至つた。 The object of the present invention is to provide a method for removing H 2 S that solves the above-mentioned drawbacks, that is, it has excellent desulfurization efficiency, can process a large amount of gas, can easily recover sulfur, does not require large-scale equipment, and is economical. The purpose of the present inventors is to provide an advantageous method for removing H 2 S, and as a result of extensive studies, the present inventors have found that H 2 S in the gas can be removed by ferric sulfate [Fe 2
(SO 4 ) 3 ] By contact reaction with an aqueous solution,
It was discovered that extremely excellent H 2 S removal efficiency was obtained, and that H 2 S removal and solid sulfur production were performed simultaneously. By using the FeSO 4 and H 2 SO 4 regenerated by the catalytic reaction, all of the objects of the present invention were achieved and the present invention was completed.
次に、本発明を図に基づいて詳細に説明を行
う。 Next, the present invention will be explained in detail based on the drawings.
図は、本発明の説明図（フローシート）であ
り、H2Sを含有する流入ガスは配管１を経て脱硫
器３１に入り、ここで配管１９より流入するFe2
（SO4）3を主成分とする脱硫用液により脱流され、
配管２から次工程（ガスホルダー又はボイラー
等）へ流出させる。 The figure is an explanatory diagram (flow sheet) of the present invention, in which the inflow gas containing H 2 S enters the desulfurizer 31 via the pipe 1, where Fe 2 flowing in from the pipe 19
It is deflowed by a desulfurization liquid mainly composed of (SO 4 ) 3 ,
It flows out from piping 2 to the next process (gas holder, boiler, etc.).
ここで脱硫用液は次式に従つてH2Sを流入ガス
から分離し、固形のＳに変換する。一方Fe2
（SO4）3は還元されFeSO4とH2SO4となる。 Here, the desulfurization liquid separates H 2 S from the incoming gas and converts it into solid S according to the following formula. On the other hand Fe 2
(SO 4 ) 3 is reduced to FeSO 4 and H 2 SO 4 .
Fe2（SO4）3＋H2S→2FeSO4
＋H2SO4＋Ｓ↓ (1)
これによつて、確実にガス中のH2Sが除去され
100％近くもの高い脱硫率が達成可能である上に、
脱硫器３１内で脱硫と固形のイオウの生成が同時
に行われ、プロセス的に非常に有利である。又、
脱硫器としては常圧式と高圧式があるが本発明に
おいては常圧式のものを使用すれば十分である。Fe 2 (SO 4 ) 3 +H 2 S→2FeSO 4 +H 2 SO 4 +S↓ (1) This ensures that H 2 S in the gas is removed.
In addition to being able to achieve a high desulfurization rate of nearly 100%,
Desulfurization and production of solid sulfur are performed simultaneously in the desulfurizer 31, which is very advantageous in terms of process. or,
There are two types of desulfurizers: normal pressure type and high pressure type, but in the present invention, it is sufficient to use the normal pressure type.
更に本発明においては、脱硫器３１内で生成す
る固形イオウを含む脱硫廃液を、プロセスのクロ
ーズド化をはかつて、有効に利用しており次にこ
の点について詳細に説明を行う。 Furthermore, in the present invention, the desulfurization waste liquid containing solid sulfur produced in the desulfurizer 31 is effectively utilized in order to make the process closed, and this point will be explained in detail next.
固形イオウを含む脱硫廃液は配管３，４を経
て、イオウ分離槽３２に流入し、ここで上澄液と
イオウ泥とに分離される。イオウ泥は配管５、ポ
ンプ４１、配管７を経て脱水機３３へ送られ、こ
こで脱水イオウと濾液とに分離される。脱水イオ
ウは工業用原料として有効利用が可能である。固
形イオウの沈降又は脱水が不良の場合には、配管
２０又は２１より凝集剤を添加する事が効果的で
ある。 The desulfurization waste liquid containing solid sulfur flows into a sulfur separation tank 32 via pipes 3 and 4, where it is separated into a supernatant liquid and sulfur mud. The sulfur mud is sent to the dehydrator 33 via the pipe 5, pump 41, and pipe 7, where it is separated into dehydrated sulfur and filtrate. Dehydrated sulfur can be effectively used as an industrial raw material. If settling or dehydration of solid sulfur is poor, it is effective to add a flocculant through pipe 20 or 21.
イオウ分離槽の上澄液は配管１０より、又濾液
混合ライン８により濾液ピツト３４へ貯蔵された
濾液は濾液ポンプ４２、配管９を経て共に酸化槽
３５に送られる。両液共、主成分はFeSO4と
H2SO4であり、PHは１〜３の酸性液である。 The supernatant liquid of the sulfur separation tank is sent to the oxidation tank 35 through the pipe 10, and the filtrate stored in the filtrate pit 34 is sent to the oxidation tank 35 through the filtrate pump 42 and the pipe 9. The main components of both liquids are FeSO 4 and
It is H 2 SO 4 and is an acidic liquid with a pH of 1 to 3.
酸化槽３５では、チオバチルス フエロオキシ
ダンス（Thiobacillus Ferrooxidans）、フエロ
バチルス フエロオキシダンス（Ferrobacillus
Ferrooxidans）、フエロバチルス スルホオキシ
ダンス（Ferrobacillus Sulfooxidans）等の鉄酸
化バクテリアの存在下で酸素源を供給する（例え
ば曝気ブロワー４３により配管１３を経て空気曝
気する。又は曝気機３９により酸素を供給する
等）事により、流入液のFeSO4とH2SO4は次式に
従つて速やかにFe2（SO4）3に酸化され、このFe2
（SO4）3は脱硫のために再利用されるものである。 In the oxidation tank 35, Thiobacillus Ferrooxidans, Ferrobacillus Ferrooxidans
Supplying an oxygen source in the presence of iron-oxidizing bacteria such as Ferrooxidans), Ferrobacillus Sulfooxidans, etc. (for example, aerating air through the pipe 13 with an aeration blower 43, or supplying oxygen with an aerator 39, etc.) As a result, FeSO 4 and H 2 SO 4 in the influent are quickly oxidized to Fe 2 (SO 4 ) 3 according to the following equation, and this Fe 2
(SO 4 ) 3 is recycled for desulfurization.
4FeSO4＋2H2SO4＋O2鉄酸化バクテリア
―――――――→
2Fe2（SO4）3＋2H2O (2)
この際、流入液にバクテリアの栄養素が不足す
る場合には、Ｎ、Ｐ、Ｋ等の栄養源を配管１１を
経て適宜添加する事が望ましい。又、酸化槽内の
バクテリア濃度を上げる事が酸化能力の増大につ
ながるが、この為バクテリアのトレーガー（例え
ば、パルプ、パルプ滓、アスベスト綿、ケイソウ
土、粉炭、粉末活性炭等）を添加ライン２２によ
り随時適当量添加する事が効果的である。4FeSO 4 +2H 2 SO 4 + O 2Iron-oxidizing bacteria――――――→ 2Fe 2 (SO 4 ) 3 +2H 2 O (2) At this time, if the influent lacks nutrients for the bacteria, N, It is desirable to add nutrients such as P and K as appropriate via piping 11. Increasing the concentration of bacteria in the oxidation tank will lead to an increase in oxidation capacity, and for this purpose, bacterial traeger (for example, pulp, pulp slag, asbestos cotton, diatomaceous earth, powdered charcoal, powdered activated carbon, etc.) is added through the addition line 22. It is effective to add an appropriate amount at any time.
(2)式で生成したFe2（SO4）3は次式により加水分
解を受け、一部が塩基性硫酸鉄Fe（OH）SO4と
なり、不溶化する。 Fe 2 (SO 4 ) 3 generated in equation (2) undergoes hydrolysis according to the following equation, and a portion becomes basic iron sulfate Fe(OH)SO 4 and becomes insolubilized.
Fe2（SO4）3＋2H2O→2Fe（OH）SO4
＋H2SO4 (3)
Fe（OH）SO4の生成率はPHと密接な関係があ
り、PHを下げる程小さくなる。Fe（OH）SO4の
フロツクはバクテリアのトレーガーとなる長所を
持つが、一方、Fe（OH）SO4の生成は脱硫用Fe2
（SO4）3の再生歩留の低下につながる。この意味
で酸化槽PHは２以下にコントロールするのが望ま
しい。なお、酸化槽内のバクテリアは、耐酸性は
もちろんのこと耐熱性にも優れているため、槽内
の温度変化の影響はほとんどない。Fe 2 (SO 4 ) 3 +2H 2 O→2Fe(OH)SO 4 +H 2 SO 4 (3) The production rate of Fe(OH)SO 4 is closely related to PH, and decreases as the PH is lowered. Fe(OH)SO 4 flocs have the advantage of being a bacterial trager, whereas Fe(OH)SO 4 production is Fe 2 for desulfurization.
This leads to a decrease in the regeneration yield of (SO 4 ) 3 . In this sense, it is desirable to control the oxidation tank pH to 2 or less. It should be noted that the bacteria in the oxidation tank have excellent not only acid resistance but also heat resistance, so they are hardly affected by temperature changes inside the tank.
酸化混合液は配管１４を経て汚泥分離槽３６に
送られ、ここで上澄の再生液と汚泥とに分離さ
れ、沈降汚泥の一部は返送汚泥ポンプ４４、配管
１５を経て酸化槽へ戻され、汚泥濃度の維持をは
かる。増殖した余剰の汚泥は配管１６を経て引き
抜かれる。 The oxidized mixed liquid is sent to the sludge separation tank 36 via the pipe 14, where it is separated into a supernatant regenerated liquid and sludge, and a part of the settled sludge is returned to the oxidation tank via the return sludge pump 44 and the pipe 15. , maintain the sludge concentration. The surplus sludge that has grown is drawn out through the pipe 16.
再生液は、再生液ピツト３７で水及びFe2
（SO4）3を添加ライン１７及び１８により補給し
て所定の量及び質に調整（ガス量、H2S濃度等で
異なる）した後、脱硫用液ポンプ４５、配管１９
を経て再び脱硫に供される。 The regenerating liquid is mixed with water and Fe 2 in the regenerating liquid pit 37.
After replenishing (SO 4 ) 3 through addition lines 17 and 18 and adjusting it to a predetermined amount and quality (varies depending on gas amount, H 2 S concentration, etc.), desulfurization liquid pump 45 and piping 19
After that, it is again subjected to desulfurization.
このように本発明は、イオウの回収が容易でプ
ロセスのクローズド化をはかつて脱硫廃液を有効
に利用し、大がかりな設備を必要とせず、ランニ
ングコストの低い経済的にも非常に有利なもので
ある。 In this way, the present invention makes it easy to recover sulfur, makes the process more closed, makes effective use of desulfurization waste liquid, does not require large-scale equipment, and is very economically advantageous with low running costs. be.
なお、補給の水及びFe2（SO4）3は配管１９の途
中に設けるラインミキサー３８にて供給しても良
い。又、脱硫廃液はイオウ分離槽３２を経ずに配
管６、ポンプ４１、配管７を経て直接脱水機３３
で固形イオウを分離しても良く、Fe2（SO4）3の損
失分を補うために相当量のFeSO4を添加ライン１
２により酸化槽３５へ供給しても良い。 Note that the makeup water and Fe 2 (SO 4 ) 3 may be supplied by a line mixer 38 provided in the middle of the pipe 19. In addition, the desulfurization waste liquid does not pass through the sulfur separation tank 32, but directly passes through the pipe 6, pump 41, and pipe 7 to the dehydrator 33.
Solid sulfur may be separated by adding a considerable amount of FeSO 4 to the addition line 1 to compensate for the loss of Fe 2 (SO 4 ) 3 .
2 may be supplied to the oxidation tank 35.
図は、本発明の説明図である。
３１……脱硫器、３２……イオウ分離器、３３
……脱水機、３４……濾液ピツト、３５……酸化
槽、３６……汚泥分離槽、３７……再生液ピツ
ト、３８……ラインミキサー、３９……曝気機。
The figure is an explanatory diagram of the present invention. 31...Desulfurizer, 32...Sulfur separator, 33
... dehydrator, 34 ... filtrate pit, 35 ... oxidation tank, 36 ... sludge separation tank, 37 ... regeneration liquid pit, 38 ... line mixer, 39 ... aeration machine.
Claims (1)
反応させて除去し、かつ、鉄酸化バクテリア及び
酸素の存在下で前記接触反応により生成する
FeSO4及びH2SO4からFe2（SO4）3水溶液を再生
し、これを再び硫化水素の除去に使用することを
特徴とする硫化水素の除去方法。1. Hydrogen sulfide in the gas is removed by a catalytic reaction with an aqueous Fe 2 (SO 4 ) 3 solution, and hydrogen sulfide is generated by the catalytic reaction in the presence of iron-oxidizing bacteria and oxygen.
A method for removing hydrogen sulfide, which comprises regenerating an aqueous Fe 2 (SO 4 ) 3 solution from FeSO 4 and H 2 SO 4 and using it again for removing hydrogen sulfide.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP57034981A JPS58152488A (en) | 1982-03-05 | 1982-03-05 | Removal of hydrogen sulfide |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP57034981A JPS58152488A (en) | 1982-03-05 | 1982-03-05 | Removal of hydrogen sulfide |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS58152488A JPS58152488A (en) | 1983-09-10 |
| JPH0218129B2 true JPH0218129B2 (en) | 1990-04-24 |
Family
ID=12429318
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP57034981A Granted JPS58152488A (en) | 1982-03-05 | 1982-03-05 | Removal of hydrogen sulfide |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS58152488A (en) |
Families Citing this family (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS6121721A (en) * | 1984-07-10 | 1986-01-30 | Dowa Mining Co Ltd | Treatment of h2s in gas |
| JPS61274724A (en) * | 1985-05-31 | 1986-12-04 | Dowa Mining Co Ltd | Treatment of malodor |
| GB8526743D0 (en) * | 1985-10-30 | 1985-12-04 | Shell Int Research | Sour gas treatment process |
| US4931262A (en) * | 1987-03-03 | 1990-06-05 | Dowa Mining Co., Ltd. | Method of treating H2 S containing gases |
| JP4869543B2 (en) * | 2003-01-31 | 2012-02-08 | 新日本製鐵株式会社 | Wastewater purification method |
| DE10340049A1 (en) * | 2003-08-28 | 2005-03-24 | Micropro Gmbh | Microbial process and plant for the purification of gases |
-
1982
- 1982-03-05 JP JP57034981A patent/JPS58152488A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS58152488A (en) | 1983-09-10 |
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