TW201414827A - Method for the removal of aromatic hydrocarbons from coke oven gas with biodiesel as a scrubbing liquid and a device for performing the method - Google Patents
Method for the removal of aromatic hydrocarbons from coke oven gas with biodiesel as a scrubbing liquid and a device for performing the method Download PDFInfo
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1487—Removing organic compounds
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- C10K1/00—Purifying combustible gases containing carbon monoxide
- C10K1/08—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors
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Abstract
Description
本發明係關於自煉焦爐氣體移除芳香烴之方法，其中生質柴油作為清洗液在迴路中傳送，其中使該煉焦爐氣體與該生質柴油在第一氣體清洗器階段中接觸並藉由吸收自該煉焦爐氣體分離芳香烴，其中隨後將富集芳香烴之該生質柴油自該第一氣體清洗器階段排出，加熱，並藉由用蒸汽汽提使芳香烴自該生質柴油部分汽提，並且其中將藉由汽提再生之該生質柴油在冷卻後至少部分地進給返回至該第一氣體清洗器。本發明之標的物亦為用於施行該方法之裝置。 The present invention relates to a method for removing aromatic hydrocarbons from a coke oven gas, wherein the raw diesel fuel is transported as a cleaning liquid in a circuit, wherein the coke oven gas is contacted with the biodiesel in a first gas scrubber stage and Absorbing aromatic hydrocarbons from the coke oven gas, wherein the biomass fuel enriched in aromatic hydrocarbons is subsequently discharged from the first gas scrubber stage, heated, and aromatic hydrocarbons are extracted from the biomass diesel portion by steam stripping Stripping, and wherein the biomass diesel regenerated by stripping is at least partially fed back to the first gas scrubber after cooling. The subject matter of the invention is also a device for carrying out the method.
芳香烴在煤煉焦期間作為新出現的煉焦爐氣體之組份而釋放。為了能夠供應芳香烴用於進一步再循環及不將其釋放至環境中，通常在自煉焦爐氣體分離焦油及氨之後在煉焦爐氣體之處理期間將芳香烴洗掉。在實踐中，使用藉由處理硬煤產生之基於焦油餾分的清洗油作為清洗液。根據主要含有之芳香烴，即苯、甲苯、間二甲苯、對二甲苯、鄰二甲苯及乙基苯，此過程步驟通常亦稱為BTEX清洗、BTX清洗或苯清洗。所述芳香烴通常亦稱為粗苯，其中粗苯之分數端視用於煉焦過程之煤及過程管控通常總計介於20克/標準立方米與40克/標準 立方米(Nm3)之間。粗苯通常包含介於55%至75%之間之苯、介於13%至19%之間之甲苯及介於5%至10%之間之二甲苯。煉焦爐氣體亦含有多環芳香烴，例如尤其萘，其在一定程度上可由清洗油吸收。煉焦爐氣體亦含有雜質，尤其H2S、HCN、NH3以及有機硫化合物。煉焦爐氣體之典型組成包含(例如)： The aromatic hydrocarbons are released as components of the newly emerging coke oven gas during coal coking. In order to be able to supply aromatic hydrocarbons for further recycling and not to release them into the environment, the aromatic hydrocarbons are typically washed off during the treatment of the coke oven gas after separation of the tar and ammonia from the coke oven gas. In practice, a tar-based cleaning oil produced by treating hard coal is used as a cleaning liquid. This process step is also commonly referred to as BTEX cleaning, BTX cleaning or benzene cleaning, depending on the predominantly aromatic hydrocarbons, namely benzene, toluene, m-xylene, p-xylene, o-xylene and ethylbenzene. The aromatic hydrocarbons are also commonly referred to as crude benzene, wherein the fraction of crude benzene is generally between 20 grams per standard cubic meter and 40 grams per standard cubic meter (Nm 3 ) depending on the coal used for the coking process and process control. . Crude benzene typically comprises between 55% and 75% benzene, between 13% and 19% toluene and between 5% and 10% xylene. The coke oven gas also contains polycyclic aromatic hydrocarbons, such as, in particular, naphthalene, which can be absorbed to some extent by the cleaning oil. The coke oven gas also contains impurities, especially H 2 S, HCN, NH 3 and organic sulfur compounds. Typical compositions of coke oven gases include, for example:
54體積%至62體積%之H2 54% to 62% by volume of H 2
23體積%至28體積%之CH4 23% to 28% by volume of CH 4
6.2體積%至8體積%之CO 6.2% by volume to 8% by volume of CO
大約7g/Nm3 H2S Approximately 7g/Nm 3 H 2 S
大約1.5g/Nm3 HCN Approximately 1.5g/Nm 3 HCN
7g/Nm3 NH3 7g/Nm 3 NH 3
大約0.5g/Nm3 SORG Approximately 0.5g/Nm 3 S ORG
至多40g/Nm3 BTX Up to 40g/Nm 3 BTX
至多2g/Nm3萘 Up to 2g/Nm 3 naphthalene
用於BTEX清洗之方法幾十年來不改變其基本特徵一直使用，且闡述於(例如)O.Grosskinsky編輯的教科書，「Handbuch des Kokereiwesens」，第2卷，1958年版本，第137頁及後續頁中。BTEX清洗在一或多個一個在另一個後面排列之清洗器中發生，其中必須確保煉焦爐氣體與作為清洗液之清洗油之間的密切接觸以由清洗油吸收芳香烴。密切接觸一方面可藉由清洗油之精細霧化且另一方面可藉由薄的油膜來達成。 The method used for BTEX cleaning has been used for decades without changing its basic characteristics, and is described, for example, in the textbook edited by O. Grosskinsky, "Handbuch des Kokereiwesens", Vol. 2, 1958 edition, page 137 and subsequent pages in. The BTEX cleaning takes place in one or more washers arranged one behind the other, in which it is necessary to ensure intimate contact between the coke oven gas and the cleaning oil as a cleaning liquid to absorb the aromatic hydrocarbons by the cleaning oil. Intimate contact can be achieved on the one hand by fine atomization of the cleaning oil and on the other hand by a thin oil film.
一方面噴灑系統與另一方面柵欄(hurdle)、襯墊(packing)或其他內置組件之組合尤其有利，其中來自噴灑系統之油滴散佈以形成具有最大可能表面之油膜。苯、甲苯及二甲苯之溶解性尤其取決於各種組份之蒸氣壓，出於此原因，將清洗油在相對低的溫度下進給至清洗器。 A combination of a spray system on the one hand and a hurdle, packing or other built-in component on the one hand is particularly advantageous, wherein oil droplets from the spray system are dispersed to form an oil film having the largest possible surface. The solubility of benzene, toluene and xylene depends inter alia on the vapor pressure of the various components, for which reason the cleaning oil is fed to the scrubber at relatively low temperatures.
另一方面，清洗油必須亦展示足夠的流動性及低黏度，以便其可容易地分佈且可形成大的表面。將在清洗器的底部收集的富集芳香烴的清洗油排出，其中隨後在升高的溫度下藉由用蒸汽汽提自清洗油汽提粗苯。隨後將清洗油在冷卻後進給返回至清洗器。為在煉焦爐氣體的通量儘可能大的情況下達成粗苯的徹底洗掉，向清洗器中添加過量的清洗油。為了能夠在現代煉焦爐中出現之煉焦爐氣體的量下實施BTEX清洗，需要大量清洗油。 On the other hand, the cleaning oil must also exhibit sufficient fluidity and low viscosity so that it can be easily distributed and can form a large surface. The aromatic hydrocarbon-enriched cleaning oil collected at the bottom of the scrubber is discharged, wherein the crude benzene is then stripped from the cleaning oil by steam stripping at elevated temperature. The cleaning oil is then fed back to the washer after cooling. In order to achieve thorough washing of the crude benzene in the case where the flux of the coke oven gas is as large as possible, an excessive amount of cleaning oil is added to the cleaner. In order to be able to perform BTEX cleaning in the amount of coke oven gas present in modern coke ovens, a large amount of cleaning oil is required.
根據KUZ’MINA E YA等人的技術文章「A NEW PETROLEUM WASH OIL TO RECOVER CRUDE BENZOL」，COKE AND CHEMISTRY U.S.S.R.，第12期，1987年，第45至49頁，提出使用化石柴油(fossil diesel oil)作為清洗液。然而，已在對應測試中確定，在用蒸汽汽提期間在由此升高之溫度下，出現橡膠樣稠度之黏性殘餘物且其在清洗油中沈澱。因此，此柴油未曾自證為迴路中之清洗液。 According to the technical article "A NEW PETROLEUM WASH OIL TO RECOVER CRUDE BENZOL" by KUZ'MINA E YA et al., COKE AND CHEMISTRY USSR, No. 12, 1987, pp. 45-49, the use of fossil diesel oil is proposed. As a cleaning solution. However, it has been determined in the corresponding tests that at the thus elevated temperature during steam stripping, a viscous residue of rubbery consistency appears and which precipitates in the cleaning oil. Therefore, this diesel has not been self-certified as a cleaning fluid in the circuit.
具有開始時所述特徵之方法自WO 2009/003 644 A1已知。為改良在BTEX清洗的背景下自煉焦爐氣體之芳香烴吸收，提出使用生質柴油作為清洗液。在本發明之範疇內，術語「生質柴油」係指有機燃料，與化石柴油相比，其並非自化石原油提取而是藉由轉酯化自植物油提取。 A method with the features described at the outset is known from WO 2009/003 644 A1. In order to improve the absorption of aromatic hydrocarbons from coke oven gas in the context of BTEX cleaning, it is proposed to use biodiesel as a cleaning liquid. Within the scope of the present invention, the term "biodiesel" refers to an organic fuel which, unlike fossil diesel, is not extracted from fossil crude oil but is extracted from vegetable oil by transesterification.
令人驚奇地，生質柴油係高度有效之清洗液，可使用其來移除芳香烴，即苯、甲苯、間二甲苯、對二甲苯、鄰二甲苯及乙基苯。此外，生質柴油價廉，易於處理，且其特徵還在於改良之CO2平衡。 Surprisingly, biodiesel is a highly effective cleaning solution that can be used to remove aromatic hydrocarbons, namely benzene, toluene, m-xylene, p-xylene, o-xylene and ethylbenzene. In addition, biodiesel is inexpensive, easy to handle, and is characterized by improved CO 2 balance.
除吸收BTEX組份以外，多環芳香烴萘之分數亦明顯降低。在根據WO 2009/003 644 A1之方法中，在標準過程參數下，萘的濃度可自通常高達2g/Nm3(克/標準立方米)之初始分數降低至100mg/Nm3至150mg/Nm3(毫克/標準立方米)之濃度。在相當的操作參數下，用基於礦物油或焦油之習用清洗液得到遠遠較高的介於200mg/Nm3與300 mg/Nm3之間之值，此乃因後者在未使用的狀態下已經具有相當大之萘殘留濃度。 In addition to the absorption of the BTEX component, the fraction of polycyclic aromatic hydrocarbon naphthalenes was also significantly reduced. In the process according to WO 2009/003 644 A1, the concentration of naphthalene can be reduced from an initial fraction of usually up to 2 g/Nm 3 (g/standard cubic meter) to 100 mg/Nm 3 to 150 mg/Nm 3 under standard process parameters. (mg/standard cubic meter) concentration. Under the equivalent operating parameters, a much higher value between 200 mg/Nm 3 and 300 mg/Nm 3 is obtained with a conventional cleaning solution based on mineral oil or tar, since the latter is in an unused state. It already has a considerable naphthalene residual concentration.
儘管生質柴油已經能夠部分移除萘，但使用根據WO 2009/003 644 A1之方法時殘存的殘留濃度仍係成問題的。除萘有害於健康及危害環境之性質以外，其亦可在佈置於BTEX清洗操作之下游之管道系統中形成沈積物，由此對應之管線受污染或可甚至被阻塞。 Although biodiesel has been able to partially remove naphthalene, the residual concentration remaining using the method according to WO 2009/003 644 A1 is still problematic. In addition to the nature of naphthalene which is detrimental to health and environmental hazards, it can also form deposits in piping systems arranged downstream of the BTEX cleaning operation, whereby the corresponding lines are contaminated or can even be blocked.
在此背景下，構成本專利申請案之基礎之問題係進一步降低經純化之煉焦爐氣體中之萘濃度。 In this context, the problem underlying the present patent application is to further reduce the concentration of naphthalene in the purified coke oven gas.
本發明之標的物及該問題之解決方案係如請求項1之方法及用於施行該方法之如請求項8之裝置。 The subject matter of the present invention and the solution to the problem are the method of claim 1 and the apparatus of claim 8 for carrying out the method.
本發明方法之特徵在於，氣體清洗操作在至少兩級中發生，其中將在第一氣體清洗器階段中純化之煉焦爐氣體傳送通過第二氣體清洗器階段以進一步移除萘，向該第二氣體清洗器階段進給第一部分量之再生生質柴油，該第一部分量與進給至第一氣體清洗器階段之第二部分量相比更徹底地汽提。 The method of the present invention is characterized in that the gas cleaning operation takes place in at least two stages, wherein the coke oven gas purified in the first gas scrubber stage is passed through a second gas scrubber stage to further remove naphthalene to the second The gas scrubber stage feeds a first portion of the regenerated biodiesel, the first portion being more thoroughly stripped than the second portion fed to the first gas scrubber stage.
作為清洗液之生質柴油通常在第一氣體清洗器階段中已經過量添加，自WO 2009/003 644 A1已知之方法亦為此情形。換言之，選擇生質柴油之吸收能力，以使得絕大部分之BTEX組份可被移除。然而，芳香烴之實際移除取決於氣相及液相中個別材料之相平衡以及清洗液與煉焦爐氣體之密切接觸。 The biodiesel as a cleaning liquid is usually already added in excess in the first gas scrubber stage, as is the case with the method known from WO 2009/003 644 A1. In other words, the absorption capacity of the biodiesel is selected so that most of the BTEX components can be removed. However, the actual removal of aromatic hydrocarbons depends on the phase equilibrium of the individual materials in the gas and liquid phases and the close contact of the cleaning fluid with the coke oven gas.
以下知識構成本發明之基礎：出於實用及經濟原因，對於BTEX清洗操作而言較佳之參數僅能夠實現萘之有限移除。具體而言，亦需要考慮到，在再生期間，藉助蒸汽來汽提芳香烴不能完全發生，此處亦應考慮再生過程期間之熱力學平衡。尤其對於萘而言，可觀察到，在習用條件下再生之清洗液展示相當大之殘留濃度，因此在氣體清洗操作期間分離萘亦相應地受到限制，尤其在較高溫度下。 The following knowledge forms the basis of the present invention: for practical and economic reasons, the preferred parameters for BTEX cleaning operations are only capable of achieving limited removal of naphthalene. In particular, it is also considered that during the regeneration, the stripping of aromatic hydrocarbons by means of steam cannot occur completely, and the thermodynamic equilibrium during the regeneration process should also be considered here. Especially for naphthalene, it has been observed that the cleaning liquor regenerated under conventional conditions exhibits a substantial residual concentration, so the separation of naphthalene during the gas cleaning operation is correspondingly limited, especially at higher temperatures.
在此背景下，尤其對於萘之移除，藉由另一再生步驟更徹底地汽提部分量之作為清洗液之生質柴油。 In this context, in particular for the removal of naphthalene, a portion of the amount of biodiesel as a cleaning liquid is more thoroughly stripped by another regeneration step.
在本發明之範疇內，基於煉焦爐氣體之通常組成，在煉焦爐氣體之氣體清洗中萘之濃度可降低至小於50mg/Nm3之濃度。 Within the scope of the present invention, the concentration of naphthalene in the gas cleaning of the coke oven gas can be reduced to a concentration of less than 50 mg/Nm 3 based on the usual composition of the coke oven gas.
根據本發明之較佳發展，作為清洗液引入第二氣體清洗器階段中之生質柴油在與先前於第一氣體清洗器階段中純化之煉焦爐氣體接觸之後自第二氣體清洗器階段部分排出，並在未再生下再次引入第二氣體清洗器階段中且由此在迴路中傳送。汽提的生質柴油之單獨迴路由此可用於第二氣體清洗器階段。始終自再生之生質柴油供應徹底汽提之第一部分量之事實防止此額外迴路中萘之過量富集。該徹底汽提之生質柴油亦可稱為超貧油，其可尤其在單獨的再生階段中獲得。 According to a preferred development of the invention, the biodiesel introduced as a cleaning liquid into the second gas scrubber stage is partially discharged from the second gas scrubber stage after contact with the coke oven gas previously purified in the first gas scrubber stage. And reintroduced into the second gas scrubber stage without regeneration and thereby transferred in the loop. A separate circuit of stripped biodiesel can thus be used in the second gas scrubber stage. The fact that the first portion of the fully self-regenerating biodiesel supply is thoroughly stripped prevents the excessive enrichment of naphthalene in this additional loop. The thoroughly stripped biodiesel may also be referred to as ultra lean oil, which may be obtained especially in a separate regeneration stage.
在第二氣體清洗器階段中，另一部分未在迴路中傳送之富集萘之生質柴油可在與煉焦爐氣體接觸之後引入第一清洗器階段中，以進一步富集芳香烴。此另一部分生質柴油之轉移有利地直接發生，即，未進一步處理。具體而言，第一氣體清洗器階段及第二氣體清洗器階段可存在於共用的氣體清洗器塔中，其中第二氣體清洗器階段佈置於第一氣體清洗器階段之上方。在該實施例之情形下，將徹底汽提之第一部分量之再生生質柴油與在氣體清洗器塔之頂部在第二再生階段中之迴路中傳送之質量流一起引入第二氣體清洗器階段中。 In the second gas scrubber stage, another portion of the naphthalene-enriched diesel fuel that is not transported in the loop may be introduced into the first scrubber stage after contact with the coke oven gas to further enrich the aromatic hydrocarbons. This transfer of another portion of the biodiesel advantageously occurs directly, ie without further processing. In particular, the first gas scrubber stage and the second gas scrubber stage may be present in a common gas scrubber column, wherein the second gas scrubber stage is disposed above the first gas scrubber stage. In the case of this embodiment, the first portion of the thoroughly stripped regenerated biomass diesel is introduced into the second gas scrubber stage along with the mass flow conveyed in the loop in the second regeneration stage at the top of the gas scrubber column. in.
吸收可以本身已知之方式藉由清洗液之分佈及/或在表面上藉由第二清洗器階段內部之內置部件來進行。在第二清洗器階段之底部，即在氣體清洗器塔之中間區域提供排放基座(discharge base)，其中在第二氣體清洗器階段中使用之呈生質柴油形式之清洗液的一部分通入佈置於其下方之第一氣體清洗器階段中，且由此與進給於其中之部分量之再生生質柴油一起進一步用於吸收BTEX組份。 The absorption can be carried out in a manner known per se by the distribution of the cleaning liquid and/or on the surface by means of built-in components inside the second washer stage. Providing a discharge base at the bottom of the second scrubber stage, ie in the middle of the gas scrubber tower, wherein a portion of the cleaning liquid in the form of biodiesel used in the second gas scrubber stage is passed It is disposed in the first gas scrubber stage below it and is thus further used to absorb the BTEX component along with a portion of the amount of regenerated biodiesel fed therein.
自第二清洗器階段轉移至另一清洗器階段中之生質柴油的量通 常對應於進給至第二氣體清洗器階段之更徹底汽提之再生生質柴油之第一部分量。 The amount of biodiesel transferred from the second scrubber stage to another scrubber stage Often corresponds to the first portion of the regenerated biodiesel that is more thoroughly stripped to the second gas scrubber stage.
在一個氣體清洗器塔中使用兩個氣體清洗器階段之較佳實施例中，富集BTEX組份及萘之生質柴油在第一氣體清洗器階段之底部(即，在氣體清洗器塔之底部)排出並供應用於再生。 In a preferred embodiment of the use of two gas scrubber stages in a gas scrubber column, the enriched BTEX component and naphthalene-based biodiesel are at the bottom of the first gas scrubber stage (ie, in the gas scrubber tower) The bottom is discharged and supplied for regeneration.
根據本發明之較佳發展，自第一氣體清洗器階段排出之生質柴油首先進給至第一再生階段進行再生，以便藉由用蒸汽(尤其用溫度高於150℃之超加熱蒸汽)汽提自生質柴油移除芳香烴。自第一再生階段排出之再生生質柴油現在總體僅具有小分數之BTEX組份，且因此可用於新的BTEX清洗操作。自第一再生階段排出之再生生質柴油因此分成第一部分量及第二部分量，其中將第二部分量再次引入第一清洗器階段中。此處通常調節至期望溫度而不進一步處理或更換清洗液。具體而言，有利的是，使第二部分量及自第一清洗器階段排出且富集芳香烴之生質柴油傳送通過常見的熱交換器。 According to a preferred development of the invention, the biomass diesel discharged from the first gas scrubber stage is first fed to the first regeneration stage for regeneration by steam (especially with superheated steam having a temperature above 150 ° C). Extraction of aromatic hydrocarbons from biodiesel. The regenerated biodiesel discharged from the first regeneration stage now generally has only a small fraction of the BTEX component and is therefore available for new BTEX cleaning operations. The regenerated biomass diesel discharged from the first regeneration stage is thus divided into a first partial amount and a second partial amount, wherein the second partial amount is reintroduced into the first scrubber stage. Here it is usually adjusted to the desired temperature without further processing or replacement of the cleaning solution. In particular, it is advantageous to pass the second partial amount and the biodiesel discharged from the first scrubber stage and enriched with aromatic hydrocarbons through a common heat exchanger.
另一方面，將第一部分量進給用於在第二再生階段中進一步再生，以便具體而言在作為清洗液之生質柴油中達成萘之進一步分離。第一部分量之分支(branching-off)有利地在藉助所述熱交換器熱回收之前進行。 On the other hand, the first partial amount is fed for further regeneration in the second regeneration stage in order to achieve further separation of the naphthalene, in particular in the biodiesel as a cleaning liquid. The branching-off of the first part is advantageously carried out before heat recovery by means of the heat exchanger.
若第一再生階段在共用再生塔內部佈置於第二再生階段之上方，會得到尤其有效之過程管控。蒸汽(尤其溫度高於150℃之超加熱蒸汽)因此首先完全引入位於再生塔之下部區域中之第二再生階段中。由於僅使第一部分量之再生生質柴油與第二再生階段中之全部蒸汽接觸，並且蒸汽仍然具有其最高溫度且先前於第一氣體清洗器階段中純化之生質柴油中芳香烴之分數總體較小，因此可有效地在第二再生階段中移除萘，使得相當大分數之萘殘留濃度得以分離。由此可得到徹底汽提之清洗液，其差不多具有新鮮生質柴油之性質，由於新鮮 生質柴油係自植物油產生，因此其首先幾乎不含萘。如上文所述，隨後將第一部分流進給至第二清洗器階段。 If the first regeneration stage is placed above the second regeneration stage within the common regeneration column, a particularly efficient process control is obtained. The steam, in particular the superheated steam having a temperature above 150 ° C, is therefore first introduced completely into the second regeneration phase in the lower region of the regeneration column. Since only a first portion of the regenerated biomass diesel is contacted with all of the steam in the second regeneration stage, and the steam still has its highest temperature and the total fraction of aromatic hydrocarbons in the biodiesel previously purified in the first gas scrubber stage It is smaller, so it is effective to remove naphthalene in the second regeneration stage, so that a considerable fraction of naphthalene residual concentration is separated. This results in a thoroughly stripped cleaning solution that has almost the same properties as fresh biodiesel due to freshness. Biomass diesel is produced from vegetable oils, so it is first almost free of naphthalene. As described above, the first portion of the stream is then fed to the second washer stage.
本發明之標的物亦係用於施行該方法之裝置，其包含第一及第二氣體清洗器階段、第一及第二再生階段、作為清洗液之生質柴油以及用以在迴路中傳送生質柴油之管線及傳送系統。 The subject matter of the present invention is also a device for performing the method, comprising first and second gas scrubber stages, first and second regeneration stages, biodiesel as a cleaning liquid, and for transporting in a loop Pipeline and conveyor system for quality diesel.
如先前上文所述，氣體清洗器階段可聯合地佈置於氣體清洗器塔中，且再生階段佈置於共用的再生塔中。 As previously described above, the gas scrubber stages can be jointly disposed in a gas scrubber column and the regeneration stage is disposed in a common regeneration column.
自根據WO 2009/003 644 A1之已知方法開始進行，在相對較低之投資成本下用本發明方法可相當大地降低萘之濃度。 Starting from the known method according to WO 2009/003 644 A1, the concentration of naphthalene can be considerably reduced by the process of the invention at relatively low investment costs.
在較佳提供之在一個氣體清洗器塔中兩個氣體清洗器階段且在一個再生塔中兩個再生階段之組合下，自煉焦爐氣體之BTEX分離及萘分離以及自作為清洗液之生質柴油之BTEX組份及萘的移除尤其有利地彼此組合，由此設備之總支出可保持較低。 BTEX separation and naphthalene separation from coke oven gas and self-cleaning as a cleaning solution, preferably in combination with two gas scrubber stages in one gas scrubber column and two regeneration stages in one regeneration column The removal of the BTEX component of the diesel and the naphthalene are particularly advantageously combined with each other, whereby the total expenditure of the equipment can be kept low.
與蒸汽一起自第一再生階段攜帶離開之芳香烴可以通常方式在下游過程中自蒸汽分離並使用。 The aromatic hydrocarbons carried away from the first regeneration stage together with the steam can be separated and used from the steam in a downstream process in the usual manner.
生質柴油係自植物油獲得。端視當地條件，典型的起始材料係(例如)菜籽油、棕櫚油、葵花籽油及大豆油，可自其形成對應的甲基酯。在本發明之範疇內，菜籽油甲基酯(RME)尤其適宜，其可在溫帶氣候區域中大量生產且可在市面上購得。 Biodiesel is obtained from vegetable oil. Depending on local conditions, typical starting materials are, for example, rapeseed oil, palm oil, sunflower oil, and soybean oil from which the corresponding methyl ester can be formed. Among the scope of the present invention, rapeseed oil methyl ester (RME) is particularly suitable, it can be produced in large quantities in temperate climate regions and is commercially available.
生質柴油之組成以及化學及物理性質闡述於(例如)DIN EN14214(2003年11月)及ASTM D 6751-07A標準中。所述標準係關於使用生質柴油作為燃料。在此背景下，對於用作清洗液來吸收芳香烴，除標準化類型之生質柴油以外，亦可使用在一定程度上偏離所述標準之生質柴油之變化形式。 The composition and chemical and physical properties of the biodiesel are described, for example, in DIN EN 14214 (November 2003) and ASTM D 6751-07A. The standard relates to the use of biodiesel as a fuel. In this context, for use as a cleaning fluid to absorb aromatic hydrocarbons, in addition to the standardized type of biodiesel, variations from biodiesel that deviate somewhat from the standard may also be used.
1‧‧‧氣體清洗器塔 1‧‧‧ gas scrubber tower
2‧‧‧再生塔 2‧‧‧Regeneration Tower
3‧‧‧第一氣體清洗器階段 3‧‧‧First gas scrubber stage
4‧‧‧第二氣體清洗器階段 4‧‧‧Second gas scrubber stage
5‧‧‧熱交換器 5‧‧‧ heat exchanger
6‧‧‧加熱裝置 6‧‧‧ heating device
7‧‧‧第一再生階段 7‧‧‧First regeneration phase
8‧‧‧第二再生階段 8‧‧‧Second regeneration phase
9‧‧‧冷卻器 9‧‧‧cooler
10‧‧‧蒸汽供應管線 10‧‧‧Steam supply pipeline
11‧‧‧單獨迴路 11‧‧‧Single loop
DK‧‧‧流速控制感測器 DK‧‧‧Flow Control Sensor
FK‧‧‧含量控制感測器 FK‧‧‧ content control sensor
TK‧‧‧溫度控制感測器 TK‧‧‧ Temperature Control Sensor
下文藉助圖式來解釋本發明，該圖式僅代表實施例之實例。該 唯一的圖在圖示(diagrammatic representation)中顯示用於自煉焦爐氣體移除芳香烴之裝置，其中生質柴油在迴路中作為清洗液傳送。 The invention is explained below with the aid of the drawings, which represent only examples of the examples. The The only diagram shows a device for the removal of aromatic hydrocarbons from coke oven gas in a diagrammatic representation in which biodiesel is delivered as a cleaning fluid in the circuit.
根據實施例之代表實例，用於自煉焦爐氣體COG移除芳香烴之設備之基本組件係氣體清洗器塔1及再生塔2。將煉焦爐氣體COG通過供應管線引入氣體清洗器塔1之下部區域中，並在垂直方向上流動通過氣體清洗器塔1，其中使其與作為清洗液之生質柴油接觸，由此芳香烴被生質柴油吸收且由此自煉焦爐氣體COG分離。隨後經純化之煉焦爐氣體COG通過氣體清洗器塔1之上部區域中之排放管線傳送離開。 According to a representative example of the embodiment, the basic components of the apparatus for removing aromatic hydrocarbons from the coke oven gas COG are the gas washer tower 1 and the regeneration tower 2. The coke oven gas COG is introduced into the lower region of the gas scrubber tower 1 through a supply line, and flows vertically through the gas scrubber tower 1 where it is brought into contact with the biomass diesel as a cleaning liquid, whereby the aromatic hydrocarbon is The biodiesel is absorbed and thus separated from the coke oven gas COG. The purified coke oven gas COG is then transported away through a discharge line in the upper region of the gas scrubber column 1.
根據本發明，在氣體清洗器塔之內部提供第一氣體清洗器階段3及位於其上方之第二氣體清洗器階段4。 According to the invention, a first gas scrubber stage 3 and a second gas scrubber stage 4 located above it are provided inside the gas scrubber tower.
富集芳香烴之作為清洗液之生質柴油自第一氣體清洗器階段3之底部(即，自氣體清洗器塔1之底部)排出，並進給至再生塔2。 The biodiesel as a cleaning liquid enriched in aromatic hydrocarbons is discharged from the bottom of the first gas scrubber stage 3 (i.e., from the bottom of the gas scrubber tower 1) and fed to the regeneration tower 2.
為能夠在第一氣體清洗器階段3中有效地移除芳香烴，即苯、甲苯、間二甲苯、對二甲苯、鄰二甲苯及乙基苯(BTEX)，在生質柴油作為清洗液之情形下較佳將溫度調節得略微高於氣體進入溫度，以避免氣體中含有的水冷凝。該溫度與再生後直接引入第一氣體清洗器階段3中之生質柴油之部分量(第二部分量)相關。 In order to be able to effectively remove aromatic hydrocarbons in the first gas scrubber stage 3, namely benzene, toluene, m-xylene, p-xylene, o-xylene and ethylbenzene (BTEX), in the production of biodiesel as a cleaning solution In this case, it is preferred to adjust the temperature slightly above the gas entry temperature to avoid condensation of water contained in the gas. This temperature is related to the partial amount (second partial amount) of the raw diesel fuel directly introduced into the first gas scrubber stage 3 after regeneration.
為能夠在再生塔2中自生質柴油分離芳香烴，提供作為清洗液之生質柴油之溫度增加，出於此目的，將自第一氣體清洗器階段3排出之生質柴油首先進給通過熱交換器5且隨後通過加熱裝置6。為調控溫度及質量流，在管線系統中提供流速控制感測器DK及溫度控制感測器TK。此外，亦可藉助含量控制感測器FK來檢測再生塔2中之含量。 In order to be able to separate the aromatic hydrocarbons from the self-generating diesel in the regeneration tower 2, the temperature increase of the biomass diesel as the cleaning liquid is provided, for which purpose the raw diesel discharged from the first gas scrubber stage 3 is first fed through the heat. The exchanger 5 and then through the heating device 6. To regulate temperature and mass flow, a flow rate control sensor DK and a temperature control sensor TK are provided in the pipeline system. Further, the content in the regeneration tower 2 can also be detected by means of the content control sensor FK.
隨後將全部生質柴油作為清洗液引入位於再生塔2之中間部分之第一再生階段7中，其中第一再生階段7中之生質柴油具有大約170℃ 至190℃之溫度。所指出之溫度範圍高於BTEX組份之沸點，因此後者自作為清洗液之生質柴油溶出。用蒸汽(尤其用溫度高於150℃之超加熱蒸汽)汽提粗苯尤其有效。大約180℃至190℃之汽提溫度尤其佳，在該溫度下作為清洗液之生質柴油不以顯著程度蒸發或分解。 Subsequently, all of the biomass diesel is introduced as a cleaning liquid into the first regeneration stage 7 located in the middle portion of the regeneration column 2, wherein the biomass diesel in the first regeneration stage 7 has a temperature of about 170 ° C. To a temperature of 190 °C. The temperature range indicated is higher than the boiling point of the BTEX component, so the latter is eluted from the biodiesel as a cleaning solution. It is especially effective to strip crude benzene with steam, especially with superheated steam at temperatures above 150 °C. The stripping temperature of about 180 ° C to 190 ° C is particularly preferred, at which temperature the biodiesel as a cleaning liquid does not evaporate or decompose to a significant extent.
隨後在第一再生階段7中純化之作為清洗液之生質柴油分成第一部分量及第二部分量。在實施例之代表實例中，清洗液在第一再生階段7之底部轉移出來並在再生塔2之外部分成第一部分量及第二部分量，其中第一部分量進給至第二再生階段8以進一步再生，而第二部分量在藉助熱交換器5及冷卻器9調節至適宜溫度後再次引入第一氣體清洗器階段3中以移除BTEX組份。 The biodiesel as a cleaning liquid purified in the first regeneration stage 7 is then divided into a first partial amount and a second partial amount. In a representative example of the embodiment, the cleaning liquid is transferred out at the bottom of the first regeneration stage 7 and is partially at the outside of the regeneration tower 2 in a first partial amount and a second partial amount, wherein the first partial amount is fed to the second regeneration stage 8 Further regeneration, while the second portion is again introduced into the first gas scrubber stage 3 after being adjusted to a suitable temperature by means of the heat exchanger 5 and the cooler 9 to remove the BTEX component.
在實施例之該代表實例之改變形式中，分成第一部分量及第二部分量亦可在第一再生階段7之底部發生，其中僅第二部分量自再生塔2轉移出來，而第一部分量直接通入第二再生階段8中以進一步純化。 In a variation of this representative example of the embodiment, the first partial amount and the second partial amount may also occur at the bottom of the first regeneration stage 7, wherein only the second partial amount is transferred from the regeneration tower 2, and the first partial amount Directly passed into the second regeneration stage 8 for further purification.
如先前上文所解釋，藉助蒸汽實施再生，該蒸汽係通過在再生塔2之下部區域中之蒸汽供應管線10引入第二再生階段8中。由於使全部蒸汽與僅總體清洗液之第一部分量接觸，並且該清洗液之此部分已經大部分經純化且該蒸汽仍然具有其初始溫度，因此可在第二再生階段8中達成生質柴油之額外純化，使得萘尤其有效地被移除。 As explained above, the regeneration is carried out by means of steam which is introduced into the second regeneration stage 8 by the steam supply line 10 in the lower region of the regeneration column 2. Since all of the steam is contacted with only a first portion of the total cleaning liquid, and this portion of the cleaning liquid has been largely purified and the steam still has its initial temperature, biodiesel can be achieved in the second regeneration stage 8. Additional purification allows the naphthalene to be removed particularly effectively.
將更徹底汽提之第一部分量之生質柴油自第二再生階段8之底部(即，自再生塔2之底部)進給至第二氣體清洗器階段4，並且與在單獨迴路11中進給至第二氣體清洗器階段4之生質柴油之部分流混合。 The first portion of the biodiesel that is more thoroughly stripped is fed from the bottom of the second regeneration stage 8 (ie, from the bottom of the regeneration column 2) to the second gas scrubber stage 4, and in the separate loop 11 A partial stream of the raw diesel fuel to the second gas scrubber stage 4 is mixed.
然而，僅一部分遞送的清洗液收集在第二氣體清洗器階段4中並在迴路中傳送，而另一部分通入佈置於第二氣體清洗器階段4之下方之第一氣體清洗器階段3中。自第二氣體清洗器階段4轉移至第一氣體清洗器階段1中之生質柴油的量對應於以徹底汽提狀態進給至第二氣 體清洗器階段4之再生生質柴油之部分量。 However, only a portion of the delivered cleaning fluid is collected in the second gas scrubber stage 4 and transported in the loop, while another portion is passed into the first gas scrubber stage 3 disposed below the second gas scrubber stage 4. The amount of biodiesel transferred from the second gas scrubber stage 4 to the first gas scrubber stage 1 corresponds to feeding to the second gas in a thorough stripping state Part of the amount of regenerated biodiesel in the body scrubber stage 4.
由於位於第二氣體清洗器階段4之該開放迴路，藉由將富集生質柴油攜帶離開至第一氣體清洗器階段3中並對應添加徹底汽提之生質柴油來避免萘濃度之增加。 Due to the open circuit at stage 2 of the second gas scrubber, the increase in naphthalene concentration is avoided by carrying the enriched biodiesel into the first gas scrubber stage 3 and correspondingly adding the thoroughly stripped biodiesel.
自作為清洗液之生質柴油汽提之BTEX組份及自清洗液汽提之萘在再生塔2之頂部離開再生塔2，並且可以本身已知之方式回收及使用。由於與先前技術相比煉焦爐氣體COG中之萘之改良分離，可防止下游管線系統中之干擾沈積物。 The BTEX component from the biodiesel stripping as a cleaning liquid and the naphthalene stripped from the cleaning liquid leave the regeneration column 2 at the top of the regeneration column 2 and can be recovered and used in a manner known per se. Due to the improved separation of naphthalene in the coke oven gas COG compared to the prior art, it is possible to prevent interference deposits in the downstream pipeline system.
調節第一氣體清洗器階段3中之過程參數，以使得BTEX組份可有效地被洗掉，而第二氣體清洗器階段4中之參數針對萘之移除最佳化。由於不同的、尤其溫度依賴性平衡，較佳在第二氣體清洗器階段4中比在第一氣體清洗器階段3中設置較高之清洗液溫度以移除萘。 The process parameters in stage 3 of the first gas scrubber are adjusted such that the BTEX component can be effectively washed away, while the parameters in the second gas scrubber stage 4 are optimized for naphthalene removal. Due to the different, especially temperature-dependent, it is preferred to set a higher cleaning liquid temperature in the second gas scrubber stage 4 than in the first gas scrubber stage 3 to remove naphthalene.
當然可在適宜時刻(未顯示)，包括在操作期間(部分)置換清洗液或加足新鮮生質柴油。 It is of course possible to replace the cleaning fluid or to add fresh biodiesel at a suitable time (not shown), including during operation (partially).
1‧‧‧氣體清洗器塔 1‧‧‧ gas scrubber tower
2‧‧‧再生塔 2‧‧‧Regeneration Tower
3‧‧‧第一氣體清洗器階段 3‧‧‧First gas scrubber stage
4‧‧‧第二氣體清洗器階段 4‧‧‧Second gas scrubber stage
5‧‧‧熱交換器 5‧‧‧ heat exchanger
6‧‧‧加熱裝置 6‧‧‧ heating device
7‧‧‧第一再生階段 7‧‧‧First regeneration phase
8‧‧‧第二再生階段 8‧‧‧Second regeneration phase
9‧‧‧冷卻器 9‧‧‧cooler
10‧‧‧蒸汽供應管線 10‧‧‧Steam supply pipeline
11‧‧‧單獨迴路 11‧‧‧Single loop
DK‧‧‧流速控制感測器 DK‧‧‧Flow Control Sensor
FK‧‧‧含量控制感測器 FK‧‧‧ content control sensor
TK‧‧‧溫度控制感測器 TK‧‧‧ Temperature Control Sensor
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| DE102012107336.8A DE102012107336A1 (en) | 2012-08-09 | 2012-08-09 | Process for the removal of aromatic hydrocarbons from Kokereigas with biodiesel as a washing liquid and apparatus for carrying out the method |
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| TW201414827A true TW201414827A (en) | 2014-04-16 |
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| EP (1) | EP2882514A1 (en) |
| AR (1) | AR092082A1 (en) |
| CA (1) | CA2881218A1 (en) |
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| AU2014390004B2 (en) * | 2014-04-09 | 2018-12-06 | Nohbell Corporation | Removal of target compounds from gases |
| CN105331395B (en) * | 2014-08-08 | 2018-02-16 | 宝钢工程技术集团有限公司 | With de- benzene heat it is oil-poor be thermal source without steam gas cleaning device and its application method |
| CN104789273A (en) * | 2015-03-27 | 2015-07-22 | 山东钢铁股份有限公司 | System for recycling coke oven raw-gas benzene substances by using raw-gas waste heat |
| CN104962322B (en) * | 2015-06-12 | 2018-05-15 | 江苏永钢集团有限公司 | Coke oven gas purification system |
| CN104962323B (en) * | 2015-06-26 | 2017-10-27 | 山东钢铁股份有限公司 | A kind of renovation process of negative pressure benzene removal circulating washing oil |
| CN109847546B (en) * | 2019-02-15 | 2021-07-27 | 邢台恒禄科技有限公司 | Environment-friendly zero-emission tail gas treatment process |
| CN113999703A (en) * | 2021-10-28 | 2022-02-01 | 宣化钢铁集团有限责任公司 | System and process for efficiently eluting benzene hydrocarbon in coke oven gas |
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| US6800120B1 (en) * | 1998-11-23 | 2004-10-05 | Fluor Corporation | Split-flow process and apparatus |
| JP4690659B2 (en) * | 2004-03-15 | 2011-06-01 | 三菱重工業株式会社 | CO2 recovery device |
| AU2007216457B2 (en) * | 2006-02-14 | 2011-02-24 | Basf Se | Refitting plants for acid gas removal |
| AR067187A1 (en) | 2007-06-29 | 2009-09-30 | Uhde Gmbh | PROCEDURE FOR SEPARATING AROMATIC HYDROCARBONS FROM GAS FROM COKE OVEN |
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| CA2881218A1 (en) | 2014-02-13 |
| WO2014023526A1 (en) | 2014-02-13 |
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| DE102012107336A1 (en) | 2014-02-13 |
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