JPWO2007108543A1 - 選択透過膜型反応器を用いた水素製造方法及び選択透過膜型反応器 - Google Patents
選択透過膜型反応器を用いた水素製造方法及び選択透過膜型反応器 Download PDFInfo
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Abstract
Description
CH4+H2O → CO+3H2 (1)
CO+H2O → CO2+H2 (2)
2CO → C+CO2 (3)
水素回収率=100×{A/(A+B)}
α={(CO2)/(CO)2}/K
β=a/b
γ=c/b
β=a/b
γ=c/b
2CO → C+CO2 (3)
水素回収率=100×{A/(A+B)}
α={(CO2)/(CO)2}/K
β=a/b
γ=c/b
図1に示すような構造を有し、βとγの値がそれぞれ下表に示す値となるような選択透過膜型反応器を作製した。分離管4は、一端部が閉じられた有底筒状のアルミナ多孔体(外径10mm、長さ75mm)からなり、その表面に選択透過膜5として、水素を選択的に透過するパラジウム−銀合金膜をメッキ法により成膜した。膜の組成は、水素透過性能を考慮してパラジウムが75質量%、銀が25質量%となるようにし、膜厚は2.5μmとした。反応管1は、両端部が開口したSUS製の円筒体で、触媒量を変えることによってβの値を変化させるため内径の異なる複数のものを使用した。改質反応触媒6には、大きさが1mm程度のペレット状に成形された市販のロジウム−アルミナ触媒又はコバルト−アルミナ触媒を使用し、反応管1と分離管4との間に充填して触媒層を形成した。
図2に示すような装置を使用し、前記実施例1〜8及び比較例1〜3の選択透過膜型反応器について、それぞれ試験を行い評価した。この装置は、原料ガス源として、エタノール、水、二酸化炭素、酸素を使用できるようライン接続され、これらを必要に応じて選択し、混合して選択透過膜型反応器に供給できるようになっている。なお、水やエタノール等の液体系の原料は気化器でガス化して供給される。
C2H5OH+3H2O → 2CO2+6H2
この反応の進行度合いを表す指標である水素変換効率は、原料のエタノール流量をC[mol/min]とし、反応で生成した水素の全流量をD[mol/min]としたとき、下記式のように定義される。
水素変換効率=100×{D/(6×C)}
ここで、反応で生成した水素の全流量Dは、選択透過膜5を透過して分離された水素の量(透過水素量)をA[ml/min]とし、選択透過膜5を透過しなかった水素の量(非透過水素量)をB[ml/min]としたとき下記式で示される。
D=A+B
Claims (7)
- 一端部がガスの入口で、他端部がガスの出口である反応管と、当該反応管内に挿入された、表面に水素を選択的に透過させる選択透過膜を有し、前記選択透過膜を透過した分離ガスの出口である排出口を有する分離管と、エタノールの改質反応を促進する改質反応触媒からなる層とを有する選択透過膜型反応器を使用し、エタノールを含む原料ガスを前記反応管の入口より供給して、触媒反応により水素、一酸化炭素及び二酸化炭素を含む混合ガスを生成し、当該混合ガスから前記選択透過膜を透過して前記分離管内に分離された水素を前記分離管の排出口より回収するとともに、前記選択透過膜を透過しない他のガス成分を前記反応管の出口から排出する水素の製造方法であって、
前記選択透過膜を透過して分離された水素の量(透過水素量)をA[ml/min]とし、前記選択透過膜を透過しなかった水素の量(非透過水素量)をB[ml/min]としたとき、下記式により定義される水素回収率の値が60〜99%となるとともに、
前記反応管の出口における二酸化炭素の分圧を(CO2)とし、前記反応管の出口における一酸化炭素の分圧を(CO)とし、前記反応管内温度における一酸化炭素の不均化反応の平衡定数をKとしたとき、下記式により定義されるαの値が0.6以上となる条件で水素の製造を行う、選択透過膜型反応器を用いた水素製造方法。
水素回収率=100×{A/(A+B)}
α={(CO2)/(CO)2}/K - 前記選択透過膜型反応器として、前記改質反応触媒からなる層の体積をa[cm3]とし、前記選択透過膜の面積をb[cm2]としたとき、下記式により定義されるβの値が0.05〜20であるような選択透過膜型反応器を使用する請求項1に記載の選択透過膜型反応器を用いた水素製造方法。
β=a/b - 前記選択透過膜型反応器として、前記改質反応触媒がFe、Co、Ni、Cu、Mo、Ru、Rh、Pd、Ag、W、Re、Os、Ir、Pt及びAuの内の少なくとも1種の金属を含有するとともに、前記金属の質量をc[mg]とし、前記選択透過膜の面積をb[cm2]としたとき、下記式により定義されるγの値が0.4〜8000であるような選択透過膜型反応器を使用する請求項1に記載の選択透過膜型反応器を用いた水素製造方法。
γ=c/b - 前記選択透過膜がPd膜又はPd合金膜であり、その膜厚が0.01〜25μmである請求項1〜3の何れか一項に記載の選択透過膜型反応器を用いた水素製造方法。
- 一端部がガスの入口で、他端部がガスの出口である反応管と、当該反応管内に挿入された、表面に水素を選択的に透過させる選択透過膜を有し、前記選択透過膜を透過した分離ガスの出口である排出口を有する分離管と、エタノールの改質反応を促進する改質反応触媒からなる層とを有する選択透過膜型反応器であって、
前記改質反応触媒からなる層の体積をa[cm3]とし、前記選択透過膜の面積をb[cm2]としたとき、下記式により定義されるβの値が0.05〜20である選択透過膜型反応器。
β=a/b - 一端部がガスの入口で、他端部がガスの出口である反応管と、当該反応管内に挿入された、表面に水素を選択的に透過させる選択透過膜を有し、前記選択透過膜を透過した分離ガスの出口である排出口を有する分離管と、エタノールの改質反応を促進する改質反応触媒からなる層とを有する選択透過膜型反応器であって、
前記改質反応触媒がFe、Co、Ni、Cu、Mo、Ru、Rh、Pd、Ag、W、Re、Os、Ir、Pt及びAuの内の少なくとも1種の金属を含有するとともに、前記金属の質量をc[mg]とし、前記選択透過膜の面積をb[cm2]としたとき、下記式により定義されるγの値が0.4〜8000である選択透過膜型反応器。
γ=c/b - 前記選択透過膜がPd膜又はPd合金膜であり、その膜厚が0.01〜25μmである請求項5又は6に記載の選択透過膜型反応器。
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