JP2012522821A - 水素を電気化学的に除去することによって、電流及び水素を発生させながら天然ガスを芳香族化合物に変換する方法 - Google Patents
水素を電気化学的に除去することによって、電流及び水素を発生させながら天然ガスを芳香族化合物に変換する方法 Download PDFInfo
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Abstract
Description
1)フィードガスの圧縮、これによって分圧は上昇する。
2)浸透側で真空を作り出すこと、又は、
3)浸透側でパージガス(Sweep-Gas)を用いること、このガスは水素分圧を低下させる。これらの手法は、機械的な応力が高い(選択肢1)及び2))か、パージガスを水素から分離する必要がある。さらに、ガス混合物を圧縮及び膨張させるための相応する装置がなければならない。動力学的な理由から、一定の割合の水素が、常に濃縮水に残る。水素透過性ポリマー膜により得られるH2/CH4混合物の透過水は例えば、通常H2分子10個に対してCH4分子を1個有する。約200℃から選択的に水素透過性になり、400〜500℃で最適な分離特性に達するPd膜の場合、透過水は通常、H2分子200個に対してCH4分子を1個有する。
a)C原子を1〜4個有する脂肪族炭化水素を少なくとも1つ含有する原料流Eを、触媒の存在下、非酸化性条件で、芳香族炭化水素及び水素を含有する生成物流Pに変換する工程、
b)前記変換の際に生じた水素の少なくとも一部を、生成物流Pから、気密な膜電極アセンブリによって電気化学的に分離する工程、ここで当該アセンブリは、プロトン選択透過性の少なくとも1つの膜と、当該膜の各側に少なくとも1つの電極触媒とを有するものであり、当該膜の濃縮側でアノード触媒によって水素の少なくとも一部を酸化してプロトンにし、当該膜を通過後にこのプロトンを、透過側でカソード触媒によって、
b1)電圧を印加して、当該プロトンの一部を還元して水素にし、
b2)電流を発生させながら、当該プロトンの一部を酸素と反応させて水にし、ここで当該酸素は、前記膜の透過側で接触させた酸素含有流Oに由来するものである、
を有するものである。
実施例1及び2では、部分工程b1)による水素分離が示されており、実施例3では、部分工程b2)による分離が示されている。
リン酸で充填されたポリベンゾイミダゾールがベースの膜を備える、活性面積が5cm2の膜電極アセンブリを使用した。この膜はCeltec P(登録商標)という名称で、BASF Fuel Cell GmbHから得られる。アノード及びカソードについてはそれぞれガス拡散電極を使用したのだが、これはELAT(登録商標)という名称で同様にBASF Fuel Cell GmbHから得られるものである。アノードもカソードも、それぞれ白金を1mg/cm2有していた。
試験パラメータ及び試験装置は、実施例1と同様だが、その違いは、カソ−ドがPtではなく、Pdを1mg/cm2含んでいたことである。その結果は表3及び表4にまとめられている。
Claims (15)
- C原子を1〜4個有する脂肪族炭化水素を、芳香族炭化水素に変換するための方法であって、以下の工程a)及びb);
a)C原子を1〜4個有する脂肪族炭化水素を少なくとも1つ含有する原料流Eを、触媒の存在下、非酸化性条件で、芳香族炭化水素及び水素を含有する生成物流Pに変換する工程、及び
b)前記変換の際に生じた水素の少なくとも一部を、生成物流Pから、気密な膜電極アセンブリによって電気化学的に分離する工程、ここで当該アセンブリは、プロトン選択透過性の少なくとも1つの膜と、当該膜の各側に少なくとも1つの電極触媒とを有するものであり、当該膜の濃縮側でアノード触媒によって水素の少なくとも一部を酸化してプロトンにし、当該プロトンが当該膜を横断後に、透過側でカソード触媒によって、
b1)電圧を印加して、当該プロトンの一部を還元して水素にし、
b2)電流を発生させながら、当該プロトンの一部を酸素と反応させて水にし、
ここで当該酸素は、前記膜の透過側で接触させた酸素含有流Oに由来するものである、
を有する、前記方法。 - 生成した芳香族炭化水素を、前記工程a)とb)との間で、又は前記工程b)の後で生成物流Pから分離することを特徴とする、請求項1に記載の方法。
- 前記生成物流Pを、水素の少なくとも一部、及び芳香族炭化水素を分離した後、前記方法に返送することを特徴とする、請求項1又は2に記載の方法。
- 前記b2)で発生した電流の少なくとも一部を、前記b1)で使用することを特徴とする、請求項1から3までのいずれか1項に記載の方法。
- 前記b1)で水素を分離するために必要な電流を、前記b2)によって発生させることを特徴とする、請求項1から4までのいずれか1項に記載の方法。
- 前記工程b)を、20〜1200℃の温度で行うことを特徴とする、請求項1から5までのいずれか1項に記載の方法。
- 前記酸素含有流Oが、酸素を少なくとも15mol%含むことを特徴とする、請求項1から6までのいずれか1項に記載の方法。
- 前記酸素含有流Oとして、空気を使用することを特徴とする、請求項1から7までのいずれか1項に記載の方法。
- 前記工程b)を、0.5〜10barの圧力で行うことを特徴とする、請求項1から8までのいずれか1項に記載の方法。
- 前記工程b)において、濃縮側と透過側に同じ圧力が存在することを特徴とする、請求項1から9までのいずれか1項に記載の方法。
- 前記工程b1)を、水素基準電極に対して0.05〜2000mVの電圧で行うことを特徴とする、請求項1から10までのいずれか1項に記載の方法。
- 前記プロトン選択透過性の膜として、ポリマー膜及びセラミック膜の群から選択される膜を使用することを特徴とする、請求項1から11までのいずれか1項に記載の方法。
- 前記電極として、ガス拡散電極を使用することを特徴とする、請求項1から12までのいずれか1項に記載の方法。
- 前記原料流Eが、メタンを少なくとも50mol%含むことを特徴とする、請求項1から13までのいずれか1項に記載の方法。
- 前記原料流Eが、天然ガスに由来することを特徴とする、請求項1から14までのいずれか1項に記載の方法。
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Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP09157397 | 2009-04-06 | ||
EP09157397.2 | 2009-04-06 | ||
PCT/EP2010/054155 WO2010115768A1 (de) | 2009-04-06 | 2010-03-30 | Verfahren zur umsetzung von erdgas zu aromaten mit elektrochemischer abtrennung von wasserstoff unter erzeugung von elektrischem strom und wasserstoff |
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JP5393872B2 (ja) | 2009-04-06 | 2014-01-22 | ビーエーエスエフ ソシエタス・ヨーロピア | 反応混合物から水素を電気化学的に分離する方法 |
EA020178B1 (ru) * | 2009-04-06 | 2014-09-30 | Басф Се | Способ превращения природного газа в ароматические углеводороды с электрохимическим отделением водорода и электрохимическим превращением водорода в воду |
PT2451770E (pt) | 2009-07-10 | 2015-03-04 | Basf Se | Processo para a aminação direta de hidrocarbonetos em amino-hidrocarbonetos com a separação eletroquímica de hidrogénio e a transformação eletroquímica do hidrogénio em água |
EP2451769B1 (de) * | 2009-07-10 | 2015-01-07 | Basf Se | Verfahren zur direktaminierung von kohlenwasserstoffen zu aminokohlenwasserstoffen mit elektrochemischer abtrennung von wasserstoff |
CN102596861B (zh) | 2009-09-03 | 2015-04-08 | 巴斯夫欧洲公司 | 从甲烷制备苯的方法 |
GB201317870D0 (en) | 2013-10-09 | 2013-11-20 | Protia As | Process for dehydroaromatization of alkanes with in-situ hydrogen removal |
EP2876097B1 (en) | 2013-11-20 | 2018-02-28 | Haldor Topsøe A/S | Process for direct conversion of a hydrocarbon-containing gas to a higher hydrocarbons product and reactor for performing the process |
CN107002260B (zh) * | 2014-09-29 | 2019-05-10 | 巴斯夫欧洲公司 | 膜电极组件,包含膜电极组件的反应器和分离氢气的方法 |
CN108270019B (zh) * | 2016-12-30 | 2020-08-07 | 中国石油天然气股份有限公司 | 一种将具有1-4个碳原子的脂肪烃转化成烯烃以及芳烃的方法 |
RU2655927C1 (ru) * | 2017-10-19 | 2018-05-30 | Федеральное государственное бюджетное учреждение науки Институт проблем переработки углеводородов Сибирского отделения Российской академии наук (ИППУ СО РАН) | Способ неокислительной конверсии метана |
US11296340B2 (en) | 2018-08-30 | 2022-04-05 | Fuelcell Energy, Inc. | Humidity transfer assemblies for fuel cells and higher-temperature electrochemical systems |
CN110483228B (zh) * | 2018-11-06 | 2022-06-28 | 中国科学院青岛生物能源与过程研究所 | 一种质子传导膜反应器中反应同时获得高纯氢气和化学品的方法和装置 |
JP2022511532A (ja) * | 2018-12-10 | 2022-01-31 | ハイドロゲン オンサイト、 エス.エル. | 天然ガス混合物から低水素含量を分離するための方法 |
US20230111285A1 (en) | 2020-03-30 | 2023-04-13 | Basf Se | Method for electrochemical hydrogen separation from natural-gas pipelines |
EP4344765A1 (en) * | 2022-09-28 | 2024-04-03 | Linde GmbH | Method and apparatus for providing a helium product |
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EA020383B1 (ru) | 2014-10-30 |
WO2010115768A1 (de) | 2010-10-14 |
EA201190238A1 (ru) | 2012-04-30 |
US8487152B2 (en) | 2013-07-16 |
US20110303550A1 (en) | 2011-12-15 |
JP5415610B2 (ja) | 2014-02-12 |
CN102365251B (zh) | 2014-01-22 |
PL2417084T3 (pl) | 2015-04-30 |
EP2417084A1 (de) | 2012-02-15 |
EP2417084B1 (de) | 2014-11-26 |
ES2529554T3 (es) | 2015-02-23 |
CN102365251A (zh) | 2012-02-29 |
KR20120027136A (ko) | 2012-03-21 |
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