JP2013527828A - 水素/合成ガス発生装置 - Google Patents
水素/合成ガス発生装置 Download PDFInfo
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Abstract
Description
a.予熱供給燃料を空気又は水蒸気又はCO2と混合して燃料混合物を得るステップ;
b.ステップ(a)で得られた燃料混合物を触媒を含む自己熱改質器中で200〜1200℃の範囲の温度で部分酸化して、H2、N2、CH4、CO、CO2からなる改質された混合物を得るステップ;
c.ステップ(b)で得られた改質された混合物をMTS/HTS水性ガスシフト反応器中で水性ガスシフト反応させ、CO含量を減少させた水素含有ガス状混合物を生成し、その後、LTS WGS中でガス状混合物を反応させて水素リッチガスを生成するステップ;
d.ステップ(c)で得られた生成ガスをPrOx反応器又はメタン化反応器中で選択的酸化させ、COのCO2への酸化によりCO2及びH2を含むガス状生成物を得るステップ;
e.ステップ(d)で得られたガス状生成物をコンデンサで冷却するステップ;
f.又はステップ(d)で得られたガス状生成物をコンデンサコイル中のCO/CO2吸収剤に任意に通過させて純H2ガスを得るステップ;
g.ステップ(e)で得られた凝縮液体を気液分離器に通過させ、ここで、液体が排水点を通過し、水素リッチガスが生成ガス出口から排出されて、燃料電池/合成ガスアプリケーションに直接供給されるステップ。
a)自己熱接触改質反応器、
b)高温又は中温水性ガスシフト反応器、
c)低温水性ガスシフト反応器、
d)選択的酸化反応器、
e)CO/CO2浄化を伴うコンデンサ及び
f)セパレータ(分離器)。
(i)ATR反応器(下部における)を含む最内シェル(I)(14)
(ii)LTS WGS反応器(上部)及び、MTS/HTS WGS反応器(下部)を含む中間シェル(M)(15)
(iii)PrOx反応器(上部)、コンデンサ(CO/CO2浄化を伴う)(中間部)及び、気液分離器(下部)を含む最外シェル(O)(16)。
シェルIとシェルMとの間の上部に位置するATR供給原料予熱部に水蒸気(水)を供給する水蒸気コイル(1)。水蒸気コイル(1)及び最内シェルの上部の壁の両方が、生成ガスから熱を吸収し、供給原料に供給し、それにより、統合型熱交換器(integrated heat exchanger)の機能を果たしている。このコイルは、水ポンプ(外部)から水を取り込み、供給原料予熱部に水蒸気を注入する。このコイルは、冷却のため又は水性ガスシフト反応における変換を増大させるために燃料発生装置内に散水する打ち抜き穴を任意に有する。
ATR用の燃料入口ポート(7a,7b,7c)、空気入口ポート及び水入口ポート
ATR後の生成したガスを測定するサンプリングポート(8)
MTS/HTS後の生成したガスを測定するサンプリングポート(9)
LTS後の生成したガスを測定するサンプリングポート(10)
PrOx後の生成したガスを測定するサンプリングポート(11)
当技術分野で公知の冷却剤/CO及び/又はCO2吸収溶液の入口(12)及び(又は)出口(13)
PO、PO+SR、PO+SR+DR、PO+DR、PO+SR+DR+WGS、PO+SR+DR+WGS+PrOx及びPO+WGS。
部分酸化を発生装置中で行わせた。メタンを燃料とした場合に起こる反応を例示する。
燃料+O2(空気)=CO+H2
CH4+0.5O2=CO+2H2(200〜1900℃)
部分酸化の後に、本明細書で例示したように水蒸気改質を発生装置中で行わせた。
燃料+O2(空気)=CO+H2
CH4+0.5O2=CO+2H2(200〜1900℃)
燃料+H2O=CO+H2 CH4+H2O=CO+3H2
燃料+H2O=CO2+H2O CH4+2H2O=CO2+4H2(200〜1600℃)
乾式改質を本明細書で例示したように行わせた。DRは、部分酸化の後に行わせ、乾式改質は、本明細書の例示のとおりである。
燃料+O2(空気)=CO+H2
CH4+0.5O2=CO+2H2(200〜1900℃)
燃料+CO2=CO+H2 CH4+CO2=2CO+2H2(200〜1600℃)
発生装置の水性ガスシフトを、部分酸化後に以下のように行わせた。
燃料+O2(空気)=CO+H2
CH4+0.5O2=CO+2H2(200〜1900℃)
CO+H2O=CO2+H2(150〜800℃)
発生装置中で行わせた選択的酸化は、以下のように示される。
CO+O2=CO2(60〜600℃)
燃料+O2(空気)=CO+H2
CH4+0.5O2=CO+2H2(200〜1900℃)
燃料+H2O=CO+H2 CH4+H2O=CO+3H2
燃料+H2O=CO2+H2O CH4+2H2O=CO2+4H2(200〜1600℃)
燃料+CO2=CO+H2
CH4+CO2=2CO+2H2(200〜1600℃)
CO+H2O=CO2+H2(120〜800℃)
部分酸化、水蒸気改質、乾式改質と続く水性ガスシフト反応を本明細書の例示のように行わせた。
部分酸化、水蒸気改質、乾式改質と続く水性ガスシフト反応、続く選択的酸化を、本明細書の例示のように行わせた。
燃料+O2(空気)=CO+H2
CH4+0.5O2=CO+2H2(200〜1900℃)
燃料+H2O=CO+H2 CH4+H2O=CO+3H2
燃料+H2O=CO2+H2O CH4+2H2O=CO2+4H2(200〜1600℃)
燃料+CO2=CO+H2
CH4+CO2=2CO+2H2(200〜1600℃)
CO+H2O=CO2+H2(120〜800℃)
CO+O2=CO2(60〜600℃)
メタンを燃料として用いる発生装置の例
ATR反応器の条件:
メタン=1分当たり2.5リットル/モル
温度=600℃及び650℃
S/C比=1.2
O2/C比=0.6
圧力=1気圧
600℃(ATR−1)及び650℃(ATR−2)のATRからの生成物
1.小型卓上水素/合成ガス発生装置
2.最大収量の水素/合成ガスの発生をもたらす様々な反応を行うことができる。
3.それを燃料電池に直接供給するためにCOのレベルを低減することができる。
4.外部熱源を必要としない。
5.供給原料及び用途に応じて、発生装置のモジュール/構成要素を選択することができる。
6.様々な単一の反応又は反応の組合せについて同じ発生装置を用いることができる。
7.水素並びに合成ガスの発生の両方に用いることができる。
Claims (17)
- 少なくとも3つの同心シェル、すなわち最内シェル、中間シェル及び最外シェルを備え、
前記最内シェル(14)は、
燃料入口ポート(7a)、空気入口ポート(7b)及び水入口ポート(7c)を経由した燃料及び空気を、水蒸気と混合するポート(6)と、
生成したガスを測定するサンプリングポート(8)とをさらに備える自己熱改質反応器から構成され、
前記中間シェル(15)は、
上部に設けられたLTS WGS反応器(低温水性ガスシフト反応器)と、
下部に設けられたMTS/HTS WGS反応器(中温/高温水性ガスシフト反応器)と、を備え、
前記LTS WGS反応器および前記MTS/HTS WGS反応器は、
前記内部シェル(14)および前記中間シェル(15)との間に配置されている水蒸気コイル(1)と、
前記MTS/HTS(15)の入口に配置されているスパージャー(3)と、
前記MTS/HTS(15)から生成したガスを測定するサンプリングポート(9)と、
前記LTS(15)から生成したガスを測定するサンプリングポート(10)と、を備え、
さらに、前記最外シェル(16)は、
上部に配置されている選択的酸化反応器(PROX)(5)と、
中間部においてCO及びCO2を浄化するコンデンサと、
下部に設けられた気液分離器と、から構成され、
前記最外シェル(16)は、さらに、
前記中間シェル(15)および前記最外シェル(16)との間に設けられたコンデンサコイル(2)と、
前記選択的酸化反応器(PROX)(5)の入口に設けられた空気スパージャー(4)と、
前記PROX(5)の後に生成したガスを測定するサンプリングポート(11)と、
冷却剤CO及びCO2吸収溶液の入口(12)及び出口(13)と、を備える、水素/合成ガス発生装置。 - 単一で小型の同心ユニットとして熱的に統合された脱硫器、自己熱反応器、水性ガスシフト反応器、選択的酸化反応器、メタン化反応器、CO及びCO2吸収器から選択される複数の反応器部を備える、請求項1に記載の発生装置。
- ATR(自己熱改質)供給原料予熱部に水蒸気を供給し、生成ガスを冷却し、水素リッチ生成ガスからCO及びCO2を吸収する複数のコイルを備える、請求項1に記載の発生装置。
- PrOx反応器(5)をメタン化反応器と置換又は併用することができる、請求項1に記載の発生装置。
- 前記発生装置の部品が、金属、セラミック、耐熱型のプラスチック、木材又は複合材料から構成されている、請求項1に記載の発生装置。
- 外部エネルギーを使用せずに用いられる、請求項1に記載の発生装置。
- 外部エネルギーを使用せずに、1モルのメタン当たり少なくとも3モルの合成ガスが発生する、請求項1に記載の発生装置。
- 熱的に常温とするか、又は発熱性燃料発生装置を脱硫器、冷却器、分離器及びCO/CO2吸収とともに協働して、熱的に均衡する化学反応の組合せを備え、
外部加熱を用いずに燃料電池及び合成ガスアプリケーションに合成ガスを直接供給する、請求項1に記載のガス発生装置。 - 前記発生装置は、PO(部分酸化)、PO+SR(水蒸気改質)、PO+SR+DR(乾式改質)、PO+DR、PO+SR+DR+WGS(水性ガスシフト)、PO+SR+DR+WGS+PrOx(選択的酸化)及びPO+WGSから選択されるが、これらに限定されない反応を組み合わせる、請求項1に記載の発生装置。
- 必要な場合、供給原料としての高温ガスを外部エネルギーとして用いることができる、請求項1に記載の発生装置。
- 請求項1に記載の発生装置中で水素ガス/合成ガスを調製する方法であって、
前記方法は、
a.予熱した供給燃料を空気又は水蒸気又はCO2と混合して燃料混合物を得るステップと、
b.ステップ(a)で得られた燃料混合物を触媒を含む自己熱改質器中で200〜1200℃の範囲の温度で部分酸化して、H2、N2、CH4、CO、CO2からなる改質された混合物を得るステップと、
c.ステップ(b)で得られた改質された混合物をMTS/HTS水性ガスシフト反応器中で水性ガスシフト反応させ、
CO含有量を減少させた水素含有ガス状混合物を生成し、
その後、LTS WGS中でガス状混合物を反応させて水素リッチガスを生成するステップと、
d.ステップ(c)で得られた生成ガスをPrOx反応器又はメタン化反応器中で選択的酸化させ、COからCO2への酸化によりCO2及びH2を含むガス状生成物を得るステップと、
e.ステップ(d)で得られたガス状生成物をコンデンサで冷却するステップと、
f.又はステップ(d)で得られたガス状生成物を前記コンデンサコイル中のCO/CO2吸収剤に任意に通過させて、純H2ガスを得るステップと、
g.ステップ(e)で得られた凝縮液体を気液分離器に通過させ、ここで、液体が前記排水点を通過し、水素リッチガスが生成ガス出口から排出されて、燃料電池/合成ガスアプリケーションに直接供給されるステップと
を含む方法。 - 前記触媒が、本明細書で述べたアルミナ担持プラチナ(Pt)、G31E(商標)、G90LDP(商標)、ATR−1、C18(商標)、G3C(商標)からなる群から選択される、請求項11に記載の方法。
- 供給燃料を生成ガスとして、再生可能又は再生不可能な脱硫触媒/吸収剤に任意に反応させる、請求項11に記載の方法。
- 使用する燃料が、メタン、液化石油ガス、炭化水素、硫黄不純物含有供給燃料、炭水化物若しくは石炭ガス化ガス、又は改質ガスを含む任意のガス(単独又はそれらの組合せ)から選択される、請求項11に記載の方法。
- ステップ(e)で使用されるCO/CO2吸収剤が、脱硫剤と混合された任意の固体及びゲル、触媒と混合された任意の固体及びゲル、触媒の前に配置された任意の固体及びゲル、触媒の後に配置された任意の固体及びゲルからなる群から選択される、請求項11に記載の方法。
- ステップ(f)における前記気液分離器の後の前記排水点で回収された液体は、適宜、再処理され、再使用され、及び/又は廃棄される、請求項11に記載の方法。
- 前記発生装置は、水素、水素リッチガス又は合成ガスを生成する、請求項1に記載のガス発生装置。
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- 2011-03-31 EP EP11724016.8A patent/EP2552580A1/en not_active Withdrawn
- 2011-03-31 KR KR1020127028569A patent/KR20130069610A/ko not_active Application Discontinuation
- 2011-03-31 JP JP2013501978A patent/JP2013527828A/ja active Pending
Also Published As
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KR20130069610A (ko) | 2013-06-26 |
CA2795015A1 (en) | 2011-10-06 |
US9126831B2 (en) | 2015-09-08 |
EP2552580A1 (en) | 2013-02-06 |
WO2011121433A1 (en) | 2011-10-06 |
AU2011234159A1 (en) | 2012-10-25 |
US20130129610A1 (en) | 2013-05-23 |
AU2011234159B2 (en) | 2016-01-21 |
CN102946987A (zh) | 2013-02-27 |
CN102946987B (zh) | 2015-02-18 |
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