JP2011525860A - Partial pump-around of carbon dioxide absorbent for cooling semi-physical physical solvents - Google Patents

Partial pump-around of carbon dioxide absorbent for cooling semi-physical physical solvents Download PDF

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JP2011525860A
JP2011525860A JP2011516360A JP2011516360A JP2011525860A JP 2011525860 A JP2011525860 A JP 2011525860A JP 2011516360 A JP2011516360 A JP 2011516360A JP 2011516360 A JP2011516360 A JP 2011516360A JP 2011525860 A JP2011525860 A JP 2011525860A
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デーヴィス，ラマー・エイ
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ユーオーピー エルエルシー
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Abstract

本発明は、合成ガス流からの、二酸化炭素および硫化水素の除去を提供する。部分的ポンプアラウンド（部分的ポンプ循環）を実施することによって、二酸化炭素吸収装置の底部から出る溶媒の一部分を冷却する。これによって溶媒循環割合および関連機器サイズを低減することが可能になる。
【選択図】図１The present invention provides for the removal of carbon dioxide and hydrogen sulfide from a synthesis gas stream. By performing a partial pump around, a portion of the solvent exiting the bottom of the carbon dioxide absorber is cooled. This makes it possible to reduce the solvent circulation rate and related equipment size.
[Selection] Figure 1

Description

本発明は、ポリエチレングリコールのジメチルエーテル（ＤＭＰＥＧ；ｄｉｍｅｔｈｙｌ ｅｔｈｅｒ ｏｆ ｐｏｌｙｅｔｈｙｌｅｎｅ ｇｌｙｃｏｌ）などの物理溶媒を使用することによって、エネルギーおよび資本必要量を低減して、汚染天然ガスまたはガス化により生じる合成ガスなどの汚染ガスを処理し、二酸化炭素および硫化水素を濃縮して除去する方法に関する。   The present invention reduces the energy and capital requirements by using a physical solvent such as dimethyl ether of polyethylene glycol (DMPEG), and pollutes such as polluted natural gas or syngas resulting from gasification. The present invention relates to a method for treating gas and concentrating and removing carbon dioxide and hydrogen sulfide.

合成ガス流から硫化水素および二酸化炭素を別々に除去するための従来技術による設計では、フラッシュ再生したセミリーン溶媒（ｓｅｍｉ−ｌｅａｎ ｓｏｌｖｅｎｔ）を、二酸化炭素吸収装置の底部と１つまたは複数の低圧フラッシュドラムとの間に循環することによって、二酸化炭素吸収装置内を流れる合成ガスから二酸化炭素を除去する。こうしたセミリーン溶媒（これは比較的少量の二酸化炭素を含む）は、このような種類の設計においては、極めて大きな流量になり得る。−３０℃（−２２°Ｆ）から１５℃（５９°Ｆ）の間の温度まで溶媒を冷却すると、溶媒容量が増加し、必要な溶媒流量が低下するが、こうした流れを低温まで直接的に冷却することは、冷却負荷が大きく、大きな機器サイズを伴うので、経済的に魅力がない。   In prior art designs for the separate removal of hydrogen sulfide and carbon dioxide from a synthesis gas stream, a flash-recycled semi-lean solvent is applied to the bottom of the carbon dioxide absorber and one or more low pressure flash drums. Is removed from the synthesis gas flowing in the carbon dioxide absorber. Such a semi-lean solvent (which contains a relatively small amount of carbon dioxide) can result in very high flow rates in this type of design. Cooling the solvent to a temperature between −30 ° C. (−22 ° F.) and 15 ° C. (59 ° F.) increases the solvent volume and reduces the required solvent flow rate, but directly reduces the flow to lower temperatures. Cooling is economically unattractive because of the large cooling load and large equipment size.

操業されている商用ユニットにおける現状のやり方では、二酸化炭素吸収装置の底部近くで全排出トレイ（全ドローオフトレー）が利用され、ここで、カラムを流下する装填溶媒（ｌｏａｄｅｄ ｓｏｌｖｅｎｔ）は、すべてカラムから排出されて、冷却交換器内にポンプ輸送され、そこで、上流の硫化水素吸収装置から出るガスと混合され、冷却された後に、二酸化炭素吸収装置の底部サンプ部分（底部排液溜め部分）に入る。こうした全排出のやり方は、二酸化炭素吸収装置の底部サンプ部分内の、装填溶媒の温度を効果的に低下させ、また、この溶媒は一連のフラッシュドラムを介してフラッシュ再生されるので、このセミリーン溶媒の温度は、溶媒からフラッシュアウトする二酸化炭素の冷却効果によってさらに低下する。こうしたセミリーン溶媒の温度が低くなることによって溶媒の二酸化炭素吸収容量が増加するので、かかる溶媒の流量を低減することができる。続く二酸化炭素のフラッシュの前に、冷却によって溶媒を冷却すると、最終のフラッシュドラムでの温度を、典型的な冷却交換器でこうした操作をしない場合に普通にみられる温度よりも低くすることが可能になる。こうした設計の欠点は、全排出トレイのために、二酸化炭素吸収装置の接線長が顕著に増加し、カラム内部のコストが増加し、専用ポンプを必要とすることによりユニット用の機器を追加させ、そして、ユニットの溶媒保有量を顕著に増加させることである。従来技術による設計では、ミキサー／交換器もやはり非常に大きく、予測可能で満足な性能を出すように設計するのが困難である。こうした従来のミキサー／交換器の運転に対する懸念も存在する。   The current practice in commercial units in operation uses a full discharge tray (full draw-off tray) near the bottom of the carbon dioxide absorber, where all the loaded solvent flowing down the column is And is pumped into a cooling exchanger where it is mixed with the gas exiting the upstream hydrogen sulfide absorber and cooled before it enters the bottom sump portion (bottom drainage reservoir portion) of the carbon dioxide absorber. enter. This total exhaust mode effectively lowers the temperature of the loading solvent in the bottom sump portion of the carbon dioxide absorber, and the solvent is flash regenerated through a series of flash drums, so the semi-lean solvent The temperature is further reduced by the cooling effect of carbon dioxide flashing out of the solvent. Since the carbon dioxide absorption capacity of the solvent is increased by lowering the temperature of the semi-lean solvent, the flow rate of the solvent can be reduced. Cooling the solvent by cooling prior to the subsequent carbon dioxide flush can reduce the temperature at the final flash drum below that normally seen without this operation on a typical cooling exchanger. become. The disadvantages of such a design are that for the entire discharge tray, the tangential length of the carbon dioxide absorber is significantly increased, the cost inside the column is increased, and the equipment for the unit is added by requiring a dedicated pump, And it is to increase the solvent holding amount of the unit remarkably. In the prior art design, the mixer / exchanger is still very large and difficult to design for predictable and satisfactory performance. There are also concerns about the operation of such conventional mixers / exchangers.

本発明は、溶媒の部分的ポンプアラウンド（ｐａｒｔｉａｌ ｐｕｍｐａｒｏｕｎｄ）に関する。   The present invention relates to a partial pumparound of the solvent.

本発明では、ポンプアラウンド（ポンプ循環）用の溶媒は、排出トレイ（ドローオフトレイ）から排出されるのではなく、カラムの底部サンプ部分（底部排液溜め部分）を出る主たる流れの支流から分割される。この装填溶媒（ｌｏａｄｅｄ ｓｏｌｖｅｎｔ）は、装填溶媒を硫化水素吸収装置へ送達するのに使用される既存のポンプを用いて、二酸化炭素吸収装置の底部からポンプ輸送され、硫化水素吸収装置に供給するのに使用される装填溶媒と共用される交換器内で冷却される。約５℃（４０°Ｆ）まで冷却された直後に、溶媒のポンプアラウンド（ポンプ循環）部分が切り離され、静的ミキサーまで送られ、ここで、硫化水素吸収装置の頂部から来るガスと混合された後に、二酸化炭素吸収装置の底部サンプ部分に輸送される。このポンプアラウンドにおける溶媒の流量は、フラッシュ再生部分の最終フラッシュドラムで所望される温度によって決定される。ポンプアラウンドの流量を増加させると、二酸化炭素吸収装置の底部温度および最終フラッシュ温度が低下することになる。−３０℃（−２２°Ｆ）もの低い温度が、ユニットで使用する冷媒の所要温度を低下させることなく、またはいかなる追加のポンプ、交換器も追加することなく、または二酸化炭素吸収装置の接線長を実質的に増加させることなく、達成することが可能である。   In the present invention, the solvent for the pump-around (pump circulation) is not discharged from the discharge tray (draw-off tray) but is divided from the main flow tributary exiting the bottom sump portion (bottom drainage reservoir portion) of the column. Is done. This loaded solvent is pumped from the bottom of the carbon dioxide absorber using the existing pump used to deliver the loaded solvent to the hydrogen sulfide absorber and is supplied to the hydrogen sulfide absorber. It is cooled in the exchanger shared with the loading solvent used in the process. Immediately after cooling to about 5 ° C. (40 ° F.), the pump-around portion of the solvent is disconnected and sent to a static mixer where it is mixed with the gas coming from the top of the hydrogen sulfide absorber. And then transported to the bottom sump portion of the carbon dioxide absorber. The solvent flow rate in this pumparound is determined by the temperature desired in the final flash drum of the flash regeneration section. Increasing the pump-around flow rate will lower the bottom temperature and the final flush temperature of the carbon dioxide absorber. Temperatures as low as −30 ° C. (−22 ° F.) do not reduce the required temperature of the refrigerant used in the unit, or add any additional pumps, exchangers, or the tangential length of the carbon dioxide absorber Can be achieved without substantially increasing.

図１は、物理溶媒を使用することによって合成ガスまたは他のガス流を処理し、二酸化炭素および硫化水素を除去し、濃縮するための流れ図を示す。   FIG. 1 shows a flow diagram for treating a synthesis gas or other gas stream by using a physical solvent to remove and concentrate carbon dioxide and hydrogen sulfide.

本発明は、物理溶媒を用いることによって、ガス流から硫化水素および二酸化炭素などの不純物を除去するものである。本発明で使用するための代表的な物理溶媒には、Ｎ−メチルピロリドン、ポリエチレングリコールのジアルキルエーテル、リン酸トリブチル、テトラメチレンスルホン、プロピレンカーボネート、メタノール、アルカノールピリジン、およびスルホラン（テトラヒドロチオフェン−１，１−ジオキシド）が含まれる。ポリプロピレングリコールのジメチルエーテルが好ましい溶媒である。   The present invention removes impurities such as hydrogen sulfide and carbon dioxide from a gas stream by using a physical solvent. Representative physical solvents for use in the present invention include N-methylpyrrolidone, dialkyl ethers of polyethylene glycol, tributyl phosphate, tetramethylene sulfone, propylene carbonate, methanol, alkanol pyridine, and sulfolane (tetrahydrothiophene-1, 1-dioxide). The preferred solvent is dimethyl ether of polypropylene glycol.

図１は、本発明の実施形態を示す。シフト反応器を通ってきた合成ガス１の流れが示され、それは、供給原料／生成物交換器４を介してライン８まで進み、次いで、溶媒を格納する硫化水素吸収装置１０の底部に入り、この溶媒は、合成ガスの流れと接触することによって硫化水素および他のイオウ化合物を除去する。流れ１２は、硫化水素吸収装置１０から出て、この流れ１２は硫化水素の濃度が増加している。次いで、流れ１２は、イオウ再生区画１４に進み、その流れから硫化水素が除去され、流れ１６として示されるように系（システム）から回収される。第２の流れ２８が示され、これは硫化水素吸収装置１０の頂部を出て、次いで、静的ミキサー３０まで進み、冷却装填溶媒流７８と混合され、次いで、合わさった流れは、ライン３２を介して二酸化炭素吸収装置３４の底部に入る。二酸化炭素が装填された溶媒流３８は、二酸化炭素吸収装置３４の底部を出て、一連のフラッシュドラム（４０、４６、５２）に続く流れ３９と、部分的ポンプアラウンド（部分的ポンプ循環）の一部分としての流れ６８とに分割される。流れ６８が示され、これは装填溶媒ポンプ７０によってライン７２へポンプ輸送され、次いで、装填溶媒冷却器７４までポンプ輸送されてライン７６に入る。流れ７６は、硫化水素吸収装置１０の頂部に入る流れ７９と、静的ミキサー３０まで行って第２の流れ２８と合わせられる流れ７８とに分割される。流れ３９が示され、これは高圧フラッシュＣＯ２フラッシュドラム４０まで進み、ライン４２は、二酸化炭素が出るところを示し、溶媒は、ライン４４を介して中圧フラッシュＣＯ２フラッシュドラム４６まで進み、二酸化炭素はライン４８から出て行く、溶媒はライン５０内を進み続けて低圧フラッシュＣＯ２フラッシュドラム５２に至り、二酸化炭素は、ライン５４に示すように出て行く。生成したセミリーン溶媒（ｓｅｍｉ−ｌｅａｎ ｓｏｌｖｅｎｔ）は、ライン５６を介してセミリーン溶媒ポンプ５８を通ってライン６０に進み、次いで、図に示したように二酸化炭素吸収装置３４まで戻る。精製された合成ガスは、二酸化炭素吸収装置３４の頂部を出て、ライン３６を介して供給原料／生成物交換器４まで進みライン６に至り、次いで、さらに所望の通りに加工される。流れ６２も示されているが、これは、イオウ再生区画１４からリーン溶媒冷却器６４を介してライン６６まで進み、次いで、二酸化炭素吸収装置３４まで進む。ライン１８は、イオウ再生区画１４からリサイクル圧縮機２０まで進み、さらにライン２２、リサイクルガス冷却器２４およびライン２６まで進み、硫化水素吸収装置１０に至る。 FIG. 1 shows an embodiment of the present invention. Shown is the flow of synthesis gas 1 through the shift reactor, which proceeds via feed / product exchanger 4 to line 8 and then enters the bottom of the hydrogen sulfide absorber 10 containing the solvent, This solvent removes hydrogen sulfide and other sulfur compounds by contact with the synthesis gas stream. Stream 12 exits hydrogen sulfide absorber 10, and this stream 12 has an increased concentration of hydrogen sulfide. Stream 12 then proceeds to sulfur regeneration section 14 where hydrogen sulfide is removed from the stream and recovered from the system as shown as stream 16. A second stream 28 is shown, which exits the top of the hydrogen sulfide absorber 10 and then proceeds to the static mixer 30 where it is mixed with the cooled charge solvent stream 78 and the combined stream is then passed through line 32. And enters the bottom of the carbon dioxide absorber 34. A solvent stream 38 loaded with carbon dioxide exits the bottom of the carbon dioxide absorber 34 and flows 39 following a series of flash drums (40, 46, 52) and a partial pump around (partial pump circulation). Divided into a stream 68 as part. A flow 68 is shown, which is pumped by line solvent pump 70 to line 72 and then pumped to line solvent cooler 74 and enters line 76. Stream 76 is divided into a stream 79 that enters the top of hydrogen sulfide absorber 10 and a stream 78 that goes to static mixer 30 and is combined with second stream 28. Stream 39 is shown, which goes to high pressure flash CO 2 flash drum 40, line 42 shows where carbon dioxide exits, and solvent goes to medium pressure flash CO 2 flash drum 46 via line 44, Carbon exits from line 48, solvent continues through line 50 to low pressure flash CO 2 flash drum 52, and carbon dioxide exits as shown in line 54. The produced semi-lean solvent proceeds through line 56 through semi-lean solvent pump 58 to line 60 and then returns to carbon dioxide absorber 34 as shown. The purified synthesis gas exits the top of the carbon dioxide absorber 34 and proceeds via line 36 to the feed / product exchanger 4 to line 6 where it is further processed as desired. A flow 62 is also shown, which proceeds from the sulfur regeneration section 14 via the lean solvent cooler 64 to the line 66 and then to the carbon dioxide absorber 34. The line 18 proceeds from the sulfur regeneration section 14 to the recycle compressor 20, further proceeds to the line 22, the recycle gas cooler 24, and the line 26, and reaches the hydrogen sulfide absorber 10.

本発明の部分的ポンプアラウンド（部分的ポンプ循環）を使用すると、このような部分的ポンプアラウンドを全く使用しない場合と比較して、セミリーン溶媒流量および関連の機器サイズを１０〜１５％低減させることが可能になる。本発明は、追加のポンプまたは問題の多い追加の交換器を必要とせずに、必要な溶媒流量が低くてもより低い温度を提供し、あるいは流量が同じ場合にはより大きい容量を提供する。   Using the partial pump around of the present invention reduces the semi-lean solvent flow rate and associated equipment size by 10-15% compared to not using such partial pump around at all. Is possible. The present invention provides a lower temperature with a lower solvent flow rate required, or a larger capacity at the same flow rate, without the need for additional pumps or problematic additional exchangers.

Claims (7)

（ａ）二酸化炭素吸収装置ユニット中にガス流を送る工程であって、ここで前記ガス流を溶媒と接触させることによって二酸化炭素を除去し、二酸化炭素含量が低下した処理ガス流および二酸化炭素含量が増加した装填溶媒流を生成させる工程；
（ｂ）前記装填溶媒流を、前記装填溶媒流の第１の部分および前記装填溶媒流の第２の部分に分割する工程；
（ｃ）前記装填溶媒流の前記第１の部分を少なくとも１つのフラッシュドラムに送ることによって、前記装填溶媒流をフラッシュ再生してセミリーン溶媒流を生成させ、次いで前記セミリーン溶媒流を、前記二酸化炭素吸収装置ユニットに戻す工程；
（ｄ）前記装填溶媒流の第２の部分を冷却することによって、冷却装填溶媒流を生成させる工程；
（ｅ）前記冷却装填溶媒流の第１の部分を、前記二酸化炭素吸収装置ユニットに戻す工程；および
（ｆ）前記冷却装填溶媒流の第２の部分を、硫化水素吸収器ユニットに送る工程；
を含む、前記ガス流を精製する方法。 (A) a process of sending a gas stream into the carbon dioxide absorber unit, wherein the gas stream is contacted with a solvent to remove carbon dioxide and reduce the carbon dioxide content and the carbon dioxide content Producing an increased charge solvent stream;
(B) dividing the charged solvent stream into a first part of the charged solvent stream and a second part of the charged solvent stream;
(C) flushing the charge solvent stream to produce a semi-lean solvent stream by sending the first portion of the charge solvent stream to at least one flash drum, and then converting the semi-lean solvent stream to the carbon dioxide Returning to the absorber unit;
(D) generating a cooled charge solvent stream by cooling a second portion of the charge solvent stream;
(E) returning a first portion of the cooled charge solvent stream to the carbon dioxide absorber unit; and (f) sending a second portion of the cool charge solvent stream to a hydrogen sulfide absorber unit;
A method for purifying the gas stream. 前記装填溶媒流の前記部分を冷却した後、前記硫化水素吸収装置ユニットからの生成物流と混合する、請求項１に記載の方法。   The method of claim 1, wherein the portion of the charge solvent stream is cooled and then mixed with the product stream from the hydrogen sulfide absorber unit. 前記セミリーン溶媒流が、冷却器または熱交換器を通過せずに前記二酸化炭素吸収装置に戻る、請求項１に記載の方法。   The method of claim 1, wherein the semi-lean solvent stream returns to the carbon dioxide absorber without passing through a cooler or heat exchanger. 前記ガス流が、合成ガス流である、請求項１に記載の方法。   The method of claim 1, wherein the gas stream is a synthesis gas stream. 前記ガス流が、天然ガス流である、請求項１に記載の方法。   The method of claim 1, wherein the gas stream is a natural gas stream. 前記装填溶媒流が、Ｎ−メチルピロリドン、ポリエチレングリコールのジアルキルエーテル、リン酸トリブチル、テトラメチレンスルホン、プロピレンカーボネート、メタノール、アルカノールピリジン、およびテトラヒドロチオフェン−１，１−ジオキシドからなる群から選択される物理溶媒を含む、請求項１に記載の方法。   The loading solvent stream is selected from the group consisting of N-methylpyrrolidone, dialkyl ether of polyethylene glycol, tributyl phosphate, tetramethylene sulfone, propylene carbonate, methanol, alkanol pyridine, and tetrahydrothiophene-1,1-dioxide. The method of claim 1 comprising a solvent. 前記装填溶媒流が、ポリプロピレングリコールのジメチルエーテルを含む、請求項６に記載の方法。   The method of claim 6, wherein the charge solvent stream comprises dimethyl ether of polypropylene glycol.
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