JP4268128B2 - 天然ガスから合成ガスを生成・分離するための装置および方法 - Google Patents
天然ガスから合成ガスを生成・分離するための装置および方法 Download PDFInfo
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Description
今やそのような要求は、天然ガスからメタノール合成ガス、アンモニア合成ガス、一酸化炭素および二酸化炭素を同時に製造するための装置を、下記の構成要素類(またはプラントユニット類)が単一の製造ラインにおいて順次直列に配設されてなることを特徴とする装置とすることによって果たされ得ることがわかった。
酸素供給下に、天然ガスを一酸化炭素、二酸化炭素、水素および水を含む合成ガス混合物に転化するための第1反応器A;
一酸化炭素から二酸化炭素への転化を制御するための第2反応器B;
所望により、生成するガス類を圧縮するための圧縮器C;
二酸化炭素を吸収し、メタノール合成用の一酸化炭素/水素混合ガスを取得するための吸収器D;および
液体窒素を導入してアンモニア合成ガスを取得し、且つ、一酸化炭素、アルゴンおよびメタンを同時に分離するための低温分離器E。
反応プロセスの概略を、図1に示す。
a) 4,000トン/日のメタノールを合成し、うち一部は酢酸の合成用に用いる。メタノール合成には、化学量数Snが2.05であり、二酸化炭素濃度が2〜3%であり、および窒素濃度が0.5%未満である合成ガスの組成が要求される。化学量数(Sn)は次の式によって計算する。
b) 同時に、上記と同じ装置で1,200トン/日の酢酸を合成するための合成ガス類を製造することができる。酢酸の合成には、メタノールおよび少なくとも98%の純度を有する一酸化炭素が要求される。
c) さらに、上記と同じ装置で4,000トン/日のアンモニアを合成するための合成ガス類が取得できるが、うち一部は尿素の合成に用いる。アンモニアの合成には、酸素濃度が10ppm未満であり、水素/窒素のモル比が3:1である水素と窒素の混合ガスが要求される。
d) そしてさらに、同じ装置で6,270トン/日の尿素を合成するための合成ガス類を取得することができる。尿素の合成には、純粋なアンモニアと98.5%を超える純度を有する二酸化炭素が要求される。
1. 反応器Aにおいて天然ガスから原料合成ガスを生成させ、圧力を約45バールに調整する。この原料合成ガスが反応器Aを出るとき、表1の2に示す組成を有する。
2. 反応器Aを出る原料合成ガスの約82%がガス流3として反応器Bを越えて案内される一方、原料合成ガスの残り約18%は反応器B内において一酸化炭素から二酸化炭素への制御された転化反応にかけられる。このガス流が反応器Bを出るとき、ガス流3と合流し、ガス流4を形成する。
3. 冷却・凝縮されるガス流4を、次に圧縮器Cにおいて約80バールまで加圧する。
4. 加圧後のこのガスを吸収器Dに供給し、二酸化炭素吸収剤が平均飽和度に達したとき、および二酸化炭素濃度が約2.2%まで下がったとき、ここで合成ガスの約43%を回収する。このときのガスはガス流6のような組成を有する。残りのガスは二酸化炭素の徹底的な除去精製を行うにあたり二度めの二酸化炭素吸収にかけて、二酸化炭素濃度が10ppm未満とする。こうして得られるガスはガス流7として低温分離器Eに供給される。
5. 低温分離器Eでは、合成ガスから一酸化炭素を分離し、分離後の一酸化炭素は酢酸合成ガス流10またはアンモニア合成ガス流11または残留ガス流(ガス流8)として利用され、ガス流8はガス流9中のメタノール合成ガスと合流する。メタン、アルゴンや一酸化炭素などの、合成ガス中の不純物ガス類は燃料ガスとして反応器Aのバーナーに供給される。
6. 吸収器Dで取得される二酸化炭素は、物質流15を経由して尿素の合成に用いる。
1.Hermann Gohna, "Concepts for Modern Methanol Plants". Proceedings of the 1997 World Methanol Conference, Tampa, Florida, USA (December 1997)
2."Gas Production", Ullmans's Encyclopedia of Industrial Chemistry, Vol. A12, VCH Verlagsgesellschaft mbh (1989)
3.Max App "Ammonia, Methanol, Hydrogen, Carbon Monoxide, Modern Production Technologies". British Sulphur Publishing ・ a Division of CRU Publishing Ltd., 31
Mount Pleasant, London WC1X 0AD. ISBN 1 873387 26 1 (published 1997)
4.Emil Supp "How to produce Methanol from Coal". Springer-Verlag (1990)
5.German Patent Application No. DE 102 26 210.1
Claims (18)
- 天然ガスからメタノール合成ガス、アンモニア合成ガス、一酸化炭素および二酸化炭素を同時に製造するための装置であって、該装置の構成全要素のうち、以下の構成要素類が単一の製造ラインにおいて順次直列に配設されてなることを特徴とする装置。
酸素供給下に、天然ガスを一酸化炭素、二酸化炭素、水素およびスチームを含む合成ガス混合物に転化するための第1反応器A;
一酸化炭素から二酸化炭素への酸化を制御するための第2反応器B;
二酸化炭素を吸収し、メタノール合成用の一酸化炭素/水素混合ガスを取得するための吸収器D;および
液体窒素を導入してアンモニア合成ガスを取得し、且つ、一酸化炭素、アルゴンおよびメタンを同時に分離するための低温分離器E、ただし、該低温分離器Eは、二酸化炭素を除去して精製される合成ガスの供給ライン、液体窒素の供給ライン、アンモニア合成ガスの取出しライン、精製された一酸化炭素の取出しライン、メタン、アルゴンおよび一酸化炭素を含む燃料ガスの取出しライン、ならびに一酸化炭素と水素を含む流体の取出しラインを有する。 - 圧縮器Cが設けられていて、該反応器AおよびBのそれぞれにおいて生成するガス類を圧縮し得るようになっており、且つ、二酸化炭素の物理的吸収または化学的吸収ができるように吸収器Dにおけるガス圧力が調整されていることを特徴とする、請求項1に記載の装置。
- 該反応器Aが、天然ガスの接触部分酸化を行わせるために、天然ガス、スチームおよび酸素の供給ラインを有することを特徴とする、請求項1または2に記載の装置。
- 該第2反応器にバイパス3が設けられていて、反応器Aで得られた合成ガス混合物の全部または一部が、該反応器Bを越えて該バイパスに案内され、合成ガス混合物の酸化の程度が制御されるように構成されていることを特徴とする、請求項1〜3のいずれかに記載の装置。
- 該吸収器Dが、合成ガス混合物の供給ライン、ならびに一酸化炭素と水素からなるメタノール合成ガスの取出しライン、二酸化炭素の取出しライン、および二酸化炭素を除去して精製される合成ガスの取出しラインを有することを特徴とする、請求項1〜4のいずれかに記載の装置。
- 該低温分離器Eから排出される一酸化炭素の一部を該メタノール合成用一酸化炭素/水素混合ガスと混合することを特徴とする、請求項1〜5のいずれかに記載の装置。
- 請求項1〜6のいずれかに記載の装置にスチームと酸素を導入することによって天然ガスからメタノール合成ガス、アンモニア合成ガス、一酸化炭素および二酸化炭素を同時に製造する方法であって、該第1反応器内における、未酸化の炭化水素に対するスチームのモル比が1.5〜3.0であることを特徴とする方法。
- 該第1反応器内における、未酸化の炭化水素に対するスチームのモル比が1.7であることを特徴とする、請求項7に記載の方法。
- 該第1反応器内における、未酸化の炭化水素に対する酸素のモル比が0.45〜0.7であることを特徴とする、請求項7または8に記載の方法。
- 該第1反応器内における、未酸化の炭化水素に対する酸素のモル比が0.52であることを特徴とする、請求項9に記載の方法。
- 天然ガスから合成ガスへの転化反応に酸化ニッケル含有触媒を用いることを特徴とする、請求項7〜10のいずれかに記載の方法。
- 天然ガスの合成ガスへの転化反応を、圧力25〜100バールで行うことを特徴とする、請求項7〜11のいずれかに記載の方法。
- 天然ガスの合成ガスへの転化反応を圧力約40バールで行うことを特徴とする、請求項12に記載の方法。
- 該第2反応器Bにおいて一酸化炭素を酸化して二酸化炭素に転化する際に、高温触媒の存在下に中間冷却を伴なう1段または2段の工程からなる方法で酸化を行うことを特徴とする、請求項7〜13のいずれかに記載の方法。
- 該反応器AおよびBにおいて取得される合成ガスを、該圧縮器Cを用いて60〜100バールの圧力に調整することを特徴とする、請求項7〜14のいずれかに記載の方法。
- 該反応器AおよびBにおいて取得される合成ガスを、該圧縮器Cを用いて80バールの圧力に調整することを特徴とする、請求項15に記載の方法。
- 該吸収器Dにおいて、合成ガスからの二酸化炭素の分離を、1段または2段以上の工程からなる化学的方法または物理的方法によって行うことを特徴とする、請求項7〜16のいずれかに記載の方法。
- 該分離器内に液体窒素を導入して合成ガスを冷却し温度を−150℃〜−200℃まで下げること、それによりメタン、アルゴンおよび一酸化炭素を該合成ガスから除去すること、および残留水素ガスに窒素を窒素/水素のモル比が3:1になるように添加してアンモニア合成ガスを取得することを特徴とする、請求項7〜17のいずれかに記載の方法。
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DE102004013539A1 (de) * | 2004-03-19 | 2005-10-06 | Lurgi Ag | Verfahren zur Koproduktion von Methanol und Ammoniak aus Erdgas |
DE102004014292A1 (de) * | 2004-03-22 | 2005-10-20 | Lurgi Ag | Koproduktion von Methanol und Ammoniak aus Erdgas |
CN1733873B (zh) * | 2004-08-11 | 2010-05-26 | 日本气体合成株式会社 | 液化石油气的制造方法 |
US20070148068A1 (en) * | 2005-12-23 | 2007-06-28 | Burgers Kenneth L | Reclaiming amines in carbon dioxide recovery |
US7437889B2 (en) * | 2006-01-11 | 2008-10-21 | Air Products And Chemicals, Inc. | Method and apparatus for producing products from natural gas including helium and liquefied natural gas |
DE102006056642A1 (de) * | 2006-11-30 | 2008-06-05 | Linde Ag | Verfahren und Vorrichtung zur Gewinnung von Produkten aus Synthesegas |
DE102007017403B4 (de) * | 2007-04-13 | 2012-05-31 | Lurgi Gmbh | Verfahren und Vorrichtung zum Herstellen von NH3-Synthesegas |
EP2199254A1 (en) * | 2008-12-11 | 2010-06-23 | BP p.l.c. | Integrated gas refinery |
EP2228358A1 (en) * | 2009-03-13 | 2010-09-15 | Methanol Casale S.A. | Recovery of CO2 in a process for synthesis of methanol |
RU2438975C1 (ru) * | 2010-07-21 | 2012-01-10 | ООО "Проектный офис" | Способ получения стехиометрической азотоводородной смеси, способ получения аммиака с ее использованием и устройства для реализации указанных способов |
RU2464296C1 (ru) * | 2011-07-07 | 2012-10-20 | Общество с ограниченной ответственностью "СинТоп" | Способ получения продукта синтеза фишера-тропша |
CN103030109A (zh) * | 2011-10-09 | 2013-04-10 | 中国石油化工股份有限公司 | 合成醋酸所需的合成气的制备方法 |
EP2771274B1 (en) * | 2011-10-26 | 2018-01-31 | Stamicarbon B.V. acting under the name of MT Innovation Center | Method for producing synthesis gas for methanol production |
FR2991442B1 (fr) * | 2012-05-31 | 2018-12-07 | L'air Liquide,Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Appareil et procede de separation cryogenique d'un melange de monoxyde de carbone et de methane ainsi que d'hydrogene et/ou d'azote |
RU2532199C1 (ru) * | 2013-06-26 | 2014-10-27 | Андрей Владиславович Курочкин | Устройство для аминовой очистки |
US9643856B2 (en) * | 2013-08-07 | 2017-05-09 | Kellogg Brown+Root LLC | Methods and systems for making ammonia in a double ammonia converter system |
CN103803492B (zh) * | 2014-02-18 | 2016-07-06 | 河南龙成煤高效技术应用有限公司 | 低温热解煤气制氢联产lng的方法 |
CN104447195B (zh) * | 2014-12-02 | 2017-02-22 | 华烁科技股份有限公司 | 一种利用电石炉尾气生产化工产品甲醇、天然气或合成油的方法 |
CN105152864B (zh) * | 2015-07-31 | 2017-09-19 | 赛鼎工程有限公司 | 一种由焦炉煤气与合成气制备低碳醇并副产天然气和液氨的工艺 |
JP6663211B2 (ja) * | 2015-12-04 | 2020-03-11 | 三菱重工エンジニアリング株式会社 | メタノール製造システム及び製造方法 |
CN108439332A (zh) * | 2018-04-19 | 2018-08-24 | 贵州赤天化桐梓化工有限公司 | 一种甲醇合成氢回收膜分离非渗透气回收的工艺方法 |
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