JP4088363B2 - Coal hydrocracking method - Google Patents
Coal hydrocracking method Download PDFInfo
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- JP4088363B2 JP4088363B2 JP02792198A JP2792198A JP4088363B2 JP 4088363 B2 JP4088363 B2 JP 4088363B2 JP 02792198 A JP02792198 A JP 02792198A JP 2792198 A JP2792198 A JP 2792198A JP 4088363 B2 JP4088363 B2 JP 4088363B2
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- gas
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Description
【0001】
【発明の属する技術分野】
本発明は、石炭を水素含有雰囲気下において急速に熱分解させて、ガス、タール、チャーを製造するための方法に関するものである。
【0002】
【従来の技術】
本発明者らは現在までに、石炭を急速に加熱し、熱分解することにより、石炭からガス、タール、チャーのような有用成分を製造するプロセスに関する提案を行っている。
例えば、特開平1−113491号公報には、石炭を気相中で、間接的に昇温された熱分解発生ガスと混合させることによって、石炭を短時間で熱分解し、石炭中の揮発分の多くをタール、ガスとして回収する技術が開示されている。また、特開平5−295371号公報には、石炭を急速熱分解して得られたチャーの一部を酸素でガス化し、その高温ガス中に微粉炭を吹き込むことによって、石炭の熱分解を行う技術が開示されている。更に、特開平6−88078号公報では、含水素物質を酸素で部分燃焼させ、雰囲気ガス中水素濃度を20%以上としたガス雰囲気中に石炭を吹き込むことによって石炭の熱分解を行い、石炭から生成するBTX(ベンゼン、トルエン、キシレン)の収率を特に増加させる技術の提案を行っている。
【0003】
また、現在までに、石炭水添ガス化または水素化熱分解と呼ばれるプロセスもいくつか提案されている。このプロセスは、石炭を高温高圧下において水素と反応させて、直接メタンをはじめとする炭化水素ガスおよびBTXをはじめとする液状炭化水素を製造することに特徴がある。
【0004】
【発明が解決しようとする課題】
特開平6−88078号公報で示されたプロセスは、雰囲気ガス中の水素濃度を高めることによって、特開平5−295371号公報におけるプロセスよりも、石炭の熱分解の結果生成するBTXの収率を増加させることに特徴がある。しかし、生成した熱分解ガスを酸素で部分燃焼するだけでは、雰囲気ガス中の水素濃度を高めるのには限界があるため、生成物として得られるBTXの収率にも限界点があった。図2に石炭水添ガス化プロセスのフローシートの一例を示す(燃料協会誌、第69巻、694ぺ一ジ、1990)。石炭水添ガス化プロセスにおいては、石炭を高温高圧かつほぼ100%近い高濃度の水素雰囲気下で熱分解を行うため、反応生成物として、メタンをはじめとする炭化水素を高濃度で含有する高カロリーガス、BTXをはじめとする軽質油成分を高収率で得ることができる。
【0005】
しかし、図2に示すように、石炭水添ガス化プロセスは、雰囲気ガスである非常に高濃度の水素ガスを精製するために、▲1▼生成した熱分解ガス中の水素のみを分離するための深冷分離装置、▲2▼チャーのガス化によって生成したガス全量を水素に転換、精製するための装置(酸性ガス除去装置、COシフト反応装置)が必要となる。従って、プロセスは非常に大がかりなものとなり、設備のイニシャルコストは莫大なものとなってしまう。
【0006】
また、石炭水添ガス化プロセスにおいて、ガス化のために必要な熱は、下記式(1)のような反応式で示されるメタンの生成熱によって供給される。
C+2H2 =CH4 +74.873kJ/mol・・・・・・(1)
しかし、文献(燃料協会誌、第69巻、707ぺ一ジ、1990)によると、水添ガス化反応器における壁からの熱損失、ベンゼンおよびキシレンの生成熱(吸熱反応)等を考慮すると、メタンの生成熱のみで反応器内を通常の水添ガス化反応に必要な800℃以上の温度レベルに保つのは困難であり、何らかの熱補給が必要であると述べられている。
【0007】
熱補給の方法としては、▲1▼ガス化後の生成ガスと水素の間で熱交換を行う方法、▲2▼ガス化反応器中に酸素を供給して、生成ガスや水素の一部を燃焼させて熱補給する方法、が挙げられている。しかし、前者の方法においては、高圧において効率良く稼働し、かつ生成ガス中のタール、BTX、水等の凝縮による能力低下のない大型の熱交換器の開発が必要であった。また、後者の方法においては、生成ガスや水素の一部が燃焼して消失するため、冷ガス効率が低下してしまうという欠点があった。
【0008】
本発明の目的は、メタンをはじめとする炭化水素ガスおよびBTXをはじめとする液状炭化水素を高い収率で製造することが可能であり、かつ設備のイニシャルコストを低減し、熱補給の必要がない高い熱効率の石炭水素化熱分解方法を提供するものである。
【0009】
【課題を解決するための手段】
本発明の石炭水素化熱分解方法は、石炭を急速に熱分解させて、ガス、タール、チャーを製造するプロセスにおいて、チャー、石炭、又はその他の炭素質原料の酸素によるガス化で生ずる高温ガス中に、水素リッチガスを混合し、水素濃度を高めたガス雰囲気中に石炭を吹き込み、石炭の急速加熱・熱分解反応を気流層で圧力10〜100atm且つ温度700〜1000℃にて行わせて熱分解ガス、タール及びチャーを生成し、当該生成物からチャーを分離後、前記熱分解ガスを精製して製品ガスとBTXとすると共に、前記タールを精製してBTXとその他液成分とし、更に、前記製品ガスの一部をシフト反応により前記水素リッチガスとして前記ガス化で生じる高温ガス中に混合する。
【0010】
【発明の実施の形態】
以下、本発明を詳細に説明する。図1に本発明の石炭水素化熱分解方法のフローシートを示す。
微粉砕した石炭は気流層型の熱分解反応器1へ導入される。熱分解反応器1では、高温ガス発生器2において発生する高温ガスおよび水素ガスとの混合ガスに石炭を混合し、熱分解することによって、熱分解反応生成物として熱分解ガス、タール、チャーが発生する。発生したチャーは、サイクロン3によってガス、タールと分離される。分離されたチャーの一部または全量は、高温ガス発生器2において酸素ガスによってガス化(部分酸化)され、高温ガス(主成分は水素および一酸化炭素)に変換される。高温ガス発生器2を熱分解反応器下部に設置することによって、高温ガスの顕熱は、放熱を最小限として効率良く、熱分解反応器1へ導入される。なお、炭種によっては、ガス化温度を制御するために、スチームをガス化剤として添加する場合もある。また、発生したチャーを他の用途に使用する場合は、チャーの代わりに石炭または他の炭素質原料を使用しても良い。
【0011】
熱分解ガスおよびタールは冷却器4によって分離される。タールは更に蒸留等の方式のタール精製器5によって、BTX、その他液成分に分離精製される。一方の熱分解ガスは、脱硫器6によって硫黄を除去した後、吸収等の方式のガス精製器7によって、BTXと製品ガスに分離精製される。
【0012】
製品ガスの一部はシフト反応器8へ導入され、下記(2)式に示す水性ガスシフト反応によって、一酸化炭素が水素および二酸化炭素へと変換され、水素リッチガスとなる。水素リッチガスは脱炭酸器9によって二酸化炭素が除去され、水素ガスとしてリサイクル利用される。
CO+H2 O=CO2 +H2 +40.3kJ/mol・・・・・・(2)
熱分解雰囲気ガス中の水素濃度は30%以上となるように、製品ガスをリサイクルするのが望ましい。リサイクルする水素ガスが増加した場合には、熱交換器10を設置して、熱分解ガスとの熱交換を実施しても良い。
【0013】
熱分解反応器1内の反応条件は、温度500〜1600℃、圧力1〜150atm 、ガス滞留時間0.01〜30sec とするが、BTXの収率を向上させるためには、特に温度700〜1000℃、圧力10〜100atm 、ガス滞留時間0.01〜5sec とするのが望ましい。
【0014】
【実施例】
図1に示したフローに従って、石炭1000kgの熱分解を実施した。熱分解反応温度を800℃、圧力を30atm 、ガス滞留時間を1sec とし、製品ガス1920Nm3 の内の1000Nm3 をリサイクルした。また、発生したチャーは、その全量を高温ガス発生器においてガス化した。
【0015】
表1に、その結果得られた熱分解反応生成物の発生量を示す。また比較例として、製品ガスのリサイクルを行わない、従来プロセスでの熱分解の結果を示す。実施例においては比較例よりもBTXの収率が大幅に増加した。また、BTX以外の液成分も大幅に増加したが、実施例におけるこれらの液成分の平均分子量が195であるのに対し、比較例では308であり、実施例の液成分の方がより軽質化が進行していた。
【0016】
【表1】
【0017】
表2に実施例と比較例における製品ガスの組成および燃焼熱を示す。実施例においては30atm の高圧ガスが発生するため、比較例の場合と比較して、特に発電用途に優れていた。また、製品ガス中のH2 /CO比が大きいため、メタノール合成等の化学原料としても好適である。
【0018】
【表2】
【0019】
【発明の効果】
本発明により、メタンをはじめとする炭化水素ガスおよびBTXをはじめとする液状炭化水素を高い収率で製造することが可能であり、かつ設備のイニシャルコストを低減し、熱補給の必要がない高い熱効率の石炭水素化熱分解方法を提供可能となる。
【図面の簡単な説明】
【図1】本発明の石炭水素化熱分解方法のフローシートである。
【図2】公知の石炭水添ガス化プロセスのフローシートである。
【符号の説明】
1 熱分解反応器
2 高温ガス発生器
3 サイクロン
4 冷却器
5 タール精製器
6 脱硫器
7 ガス精製器
8 シフト反応器
9 脱炭酸器
10 熱交換器[0001]
BACKGROUND OF THE INVENTION
The present invention relates to a process for producing gas, tar and char by rapidly pyrolyzing coal in a hydrogen-containing atmosphere.
[0002]
[Prior art]
To date, the present inventors have proposed a process for producing useful components such as gas, tar and char from coal by rapidly heating and pyrolyzing the coal.
For example, in Japanese Patent Laid-Open No. 1-113491, coal is pyrolyzed in a short time by mixing coal with a pyrolysis gas that has been indirectly heated in the gas phase, and the volatile matter in the coal. A technique for recovering most of these as tar and gas is disclosed. Japanese Patent Laid-Open No. 5-295371 discloses that coal is pyrolyzed by gasifying a part of char obtained by rapid pyrolysis of coal with oxygen and blowing pulverized coal into the high-temperature gas. Technology is disclosed. Furthermore, in Japanese Patent Laid-Open No. 6-88078, coal is thermally decomposed by partially burning a hydrogen-containing substance with oxygen and blowing coal into a gas atmosphere in which the hydrogen concentration in the atmosphere gas is 20% or more. Proposals have been made for a technique for particularly increasing the yield of BTX (benzene, toluene, xylene) produced.
[0003]
To date, several processes called coal hydrogenation gasification or hydropyrolysis have been proposed. This process is characterized in that coal is reacted with hydrogen under high temperature and high pressure to directly produce hydrocarbon gas including methane and liquid hydrocarbon including BTX.
[0004]
[Problems to be solved by the invention]
The process shown in Japanese Patent Laid-Open No. 6-88078 has a higher yield of BTX produced as a result of coal pyrolysis than the process in Japanese Patent Laid-Open No. 5-295371 by increasing the hydrogen concentration in the atmospheric gas. It is characterized by increasing. However, there is a limit in the yield of BTX obtained as a product because there is a limit in increasing the hydrogen concentration in the atmospheric gas only by partially burning the generated pyrolysis gas with oxygen. FIG. 2 shows an example of a flow sheet for the coal hydrogasification process (Journal of Fuel Association, Vol. 69, page 694, 1990). In the coal hydrogenation gasification process, coal is thermally decomposed in a high-temperature, high-pressure and nearly 100% high-concentration hydrogen atmosphere, so that a high concentration of hydrocarbons such as methane is contained as a reaction product. Light oil components including caloric gas and BTX can be obtained in high yield.
[0005]
However, as shown in FIG. 2, in the coal hydrogenation gasification process, in order to purify very high concentration hydrogen gas, which is an atmospheric gas, (1) only hydrogen in the generated pyrolysis gas is separated. (2) A device for converting and purifying the total amount of gas generated by gasification of char to hydrogen (an acid gas removal device, a CO shift reaction device) is required. Therefore, the process becomes very large and the initial cost of the equipment becomes enormous.
[0006]
In the coal hydrogenation gasification process, the heat required for gasification is supplied by the heat of formation of methane represented by the following reaction formula (1).
C + 2H 2 = CH 4 +74.873 kJ / mol (1)
However, according to the literature (Journal of Fuel Association, Vol. 69, page 707, 1990), considering heat loss from the walls in the hydrogenation gasification reactor, heat of formation of benzene and xylene (endothermic reaction), etc., It is stated that it is difficult to keep the inside of the reactor at a temperature level of 800 ° C. or higher, which is necessary for a normal hydrogenation gasification reaction, only with the heat of formation of methane, and some kind of heat supply is required.
[0007]
As a heat supply method, (1) a method in which heat is exchanged between the gasified product gas and hydrogen, (2) oxygen is supplied into the gasification reactor, and a part of the product gas or hydrogen is removed. And a method of replenishing heat by burning. However, in the former method, it was necessary to develop a large-sized heat exchanger that operates efficiently at high pressure and does not deteriorate in capacity due to condensation of tar, BTX, water, etc. in the product gas. Further, the latter method has a drawback in that cold gas efficiency is lowered because part of the generated gas and hydrogen is burned and lost.
[0008]
The object of the present invention is to produce hydrocarbon gas such as methane and liquid hydrocarbon such as BTX in high yield, reduce the initial cost of equipment, and need to replenish heat. There is no high thermal efficiency coal hydropyrolysis process.
[0009]
[Means for Solving the Problems]
The coal hydrogenation pyrolysis method of the present invention is a high-temperature gas generated by gasification of char, coal, or other carbonaceous raw material with oxygen in a process of rapidly pyrolyzing coal to produce gas, tar, or char. Inside, a hydrogen rich gas is mixed and coal is blown into a gas atmosphere in which the hydrogen concentration is increased, and the coal is rapidly heated and thermally decomposed at a pressure of 10 to 100 atm and a temperature of 700 to 1000 ° C. in a gas stream. Generating cracked gas, tar and char, separating char from the product, purifying the pyrolysis gas to product gas and BTX, purifying the tar to BTX and other liquid components, A part of the product gas is mixed as a hydrogen-rich gas into the high-temperature gas generated by the gasification by a shift reaction.
[0010]
DETAILED DESCRIPTION OF THE INVENTION
Hereinafter, the present invention will be described in detail. FIG. 1 shows a flow sheet of the coal hydrogenation pyrolysis method of the present invention.
The finely pulverized coal is introduced into a gas-flow-type pyrolysis reactor 1. In the pyrolysis reactor 1, coal is mixed with the mixed gas of the high-temperature gas and hydrogen gas generated in the high-
[0011]
The pyrolysis gas and tar are separated by the cooler 4. The tar is further separated and purified into BTX and other liquid components by a tar purifier 5 such as distillation. One pyrolysis gas, after removing sulfur by the desulfurizer 6, is separated and purified into BTX and product gas by a
[0012]
A part of the product gas is introduced into the
CO + H 2 O = CO 2 + H 2 +40.3 kJ / mol (2)
It is desirable to recycle the product gas so that the hydrogen concentration in the pyrolysis atmosphere gas is 30% or more. When the hydrogen gas to be recycled increases, the
[0013]
The reaction conditions in the pyrolysis reactor 1 are a temperature of 500 to 1600 ° C., a pressure of 1 to 150 atm, and a gas residence time of 0.01 to 30 seconds. In order to improve the yield of BTX, a temperature of 700 to 1000 is particularly preferred. It is desirable that the temperature is 10 ° C., the pressure is 10 to 100 atm, and the gas residence time is 0.01 to 5 seconds.
[0014]
【Example】
According to the flow shown in FIG. 1, 1000 kg of coal was pyrolyzed. The pyrolysis reaction temperature was 800 ° C., the pressure was 30 atm, the gas residence time was 1 sec, and 1000 Nm 3 of the product gas 1920 Nm 3 was recycled. Further, the generated char was gasified in a high temperature gas generator.
[0015]
Table 1 shows the amount of pyrolysis reaction products generated as a result. Further, as a comparative example, the result of thermal decomposition in a conventional process in which product gas is not recycled is shown. In the examples, the yield of BTX was significantly increased as compared with the comparative examples. In addition, the liquid components other than BTX increased significantly, but the average molecular weight of these liquid components in the examples was 195, whereas in the comparative example, it was 308, and the liquid components of the examples were lighter. Was progressing.
[0016]
[Table 1]
[0017]
Table 2 shows the composition of the product gas and the heat of combustion in the examples and comparative examples. In the examples, 30 atm of high-pressure gas was generated, so that it was particularly excellent in power generation applications as compared with the comparative example. Further, since the H 2 / CO ratio in the product gas is large, it is also suitable as a chemical raw material for methanol synthesis and the like.
[0018]
[Table 2]
[0019]
【The invention's effect】
According to the present invention, it is possible to produce hydrocarbon gas including methane and liquid hydrocarbon including BTX with high yield, and the initial cost of the equipment is reduced, and there is no need for heat supply. It becomes possible to provide a thermal hydrogenation pyrolysis method with high efficiency.
[Brief description of the drawings]
FIG. 1 is a flow sheet of a coal hydrogenation pyrolysis method of the present invention.
FIG. 2 is a flow sheet of a known coal hydrogenation gasification process.
[Explanation of symbols]
DESCRIPTION OF SYMBOLS 1
Claims (1)
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JP02792198A JP4088363B2 (en) | 1998-02-10 | 1998-02-10 | Coal hydrocracking method |
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JP02792198A JP4088363B2 (en) | 1998-02-10 | 1998-02-10 | Coal hydrocracking method |
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JP4863889B2 (en) * | 2007-01-16 | 2012-01-25 | 新日鉄エンジニアリング株式会社 | Coal hydrocracking process |
JP4906519B2 (en) * | 2007-01-16 | 2012-03-28 | 新日鉄エンジニアリング株式会社 | Coal hydrocracking process |
JP2009298909A (en) * | 2008-06-12 | 2009-12-24 | Nippon Steel Engineering Co Ltd | Utilizing method of pyrolysis char as carbonaceous material for sintering |
JP5316948B2 (en) * | 2008-10-14 | 2013-10-16 | Jfeエンジニアリング株式会社 | Biomass pyrolysis equipment |
CN101984021B (en) * | 2010-10-26 | 2011-08-10 | 西峡龙成特种材料有限公司 | Heating gas circulating type coal substance decomposing equipment |
JP6293472B2 (en) * | 2013-12-13 | 2018-03-14 | 三菱日立パワーシステムズ株式会社 | Hydrogen production apparatus and hydrogen production method |
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