JP4334577B2 - 吸収材の再生方法 - Google Patents
吸収材の再生方法 Download PDFInfo
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- JP4334577B2 JP4334577B2 JP2007060661A JP2007060661A JP4334577B2 JP 4334577 B2 JP4334577 B2 JP 4334577B2 JP 2007060661 A JP2007060661 A JP 2007060661A JP 2007060661 A JP2007060661 A JP 2007060661A JP 4334577 B2 JP4334577 B2 JP 4334577B2
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- carbon dioxide
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- 230000002745 absorbent Effects 0.000 title claims description 91
- 239000002250 absorbent Substances 0.000 title claims description 91
- 239000000463 material Substances 0.000 title claims description 53
- 238000000034 method Methods 0.000 title claims description 25
- 238000004064 recycling Methods 0.000 title 1
- 239000007789 gas Substances 0.000 claims description 97
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 79
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 68
- 238000002407 reforming Methods 0.000 claims description 36
- 239000001569 carbon dioxide Substances 0.000 claims description 34
- 229910002092 carbon dioxide Inorganic materials 0.000 claims description 34
- 238000012545 processing Methods 0.000 claims description 32
- 239000002994 raw material Substances 0.000 claims description 28
- 239000003054 catalyst Substances 0.000 claims description 25
- 239000001257 hydrogen Substances 0.000 claims description 24
- 229910052739 hydrogen Inorganic materials 0.000 claims description 24
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 23
- PAZHGORSDKKUPI-UHFFFAOYSA-N lithium metasilicate Chemical compound [Li+].[Li+].[O-][Si]([O-])=O PAZHGORSDKKUPI-UHFFFAOYSA-N 0.000 claims description 22
- 229910052912 lithium silicate Inorganic materials 0.000 claims description 21
- 238000000629 steam reforming Methods 0.000 claims description 19
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 15
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- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 52
- 229910002091 carbon monoxide Inorganic materials 0.000 description 52
- 238000011069 regeneration method Methods 0.000 description 40
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- 229910052799 carbon Inorganic materials 0.000 description 29
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 28
- 235000019441 ethanol Nutrition 0.000 description 26
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 20
- 238000010521 absorption reaction Methods 0.000 description 19
- 229910001873 dinitrogen Inorganic materials 0.000 description 14
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 14
- 238000010438 heat treatment Methods 0.000 description 13
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- 238000004519 manufacturing process Methods 0.000 description 7
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 6
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- 230000000052 comparative effect Effects 0.000 description 5
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- 229910004283 SiO 4 Inorganic materials 0.000 description 2
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
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- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 1
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
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- 239000010419 fine particle Substances 0.000 description 1
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- 229910052734 helium Inorganic materials 0.000 description 1
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 230000005764 inhibitory process Effects 0.000 description 1
- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 description 1
- 239000000395 magnesium oxide Substances 0.000 description 1
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- 238000012360 testing method Methods 0.000 description 1
- YTZVWGRNMGHDJE-UHFFFAOYSA-N tetralithium;silicate Chemical compound [Li+].[Li+].[Li+].[Li+].[O-][Si]([O-])([O-])[O-] YTZVWGRNMGHDJE-UHFFFAOYSA-N 0.000 description 1
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Description
また、最近では植物から製造される再生可能エネルギーとして注目されるエタノール(C2H5OH)を原料として水素を製造する検討も行われている(非特許文献1参照)。エタノールを原料とする水蒸気改質反応は、下記式(2)で表される。
これら反応は、副生成物が多く発生し、メタン、一酸化炭素(CO)、二酸化炭素(CO2)等の不純物が生成ガスに含有される。特に、水蒸気改質反応直後の生成ガス中には反応条件や原料により異なるものの、数体積%から数10体積%との一酸化炭素が含有される。このため、反応管の下流側に一酸化炭素(CO)変成器を接続するのが一般的である(非特許文献2参照)。CO変成器により処理された生成ガスは、一酸化炭素濃度が約0.5体積%に低下し、その後にガス精製工程に供給される。
前記式(3)において、右向きの反応が起きればCO2はリチウムシリケートと反応して吸収される。非特許文献3〜5に記載のようにメタン及びエタノールでは高温水蒸気との反応に対する平衡のシフト効果が実験により確認され、水素生成が促進されるとともに副生成物である一酸化炭素濃度が下がることが明らかにされている。
前記反応は平衡上、雰囲気中のCO2濃度が高い方が炭素の除去に有利に働く。しかしながら、前述した吸収材からのCO2放出を考慮すると、CO2放出条件と反対になる。本発明者らは、リチウムシリケートからなる吸収材を50体積%の二酸化炭素雰囲気下で650℃にて加熱した実験において、CO2が放出されず、再生が困難であることを確認した。
F.Frusteri et al., Journal of Power Sources, 132, 139 (2004) 工業調査会「水素エネルギー最前線」(2003)36ページ 特開平9−147821号公報
前記改質器内の温度を625℃以上に設定し、かつ不活性ガスまたは二酸化炭素を5体積%以下含む不活性ガスを処理ガスとして前記改質器内に前記原料ガスおよび水蒸気の供給方向と向きが反対になるよう前記排出部を通して供給することを特徴とする吸収材の再生方法が提供される。
前記上部円板状蓋体5におけるガス導入管4の開口部および前記下部円板状蓋体7における生成ガス排出管6の開口部には、メッシュ8,9がそれぞれ取り付けられている。改質用触媒10およびリチウムシリケートを含む二酸化炭素を吸収するための吸収材11は、反応管3内に充填されている。
前述した図1に示す改質器1の反応管3(内径0.02m、高さは0.9m)内に改質用触媒10gおよび吸収材60gを混合して高さが0.3mとなるように充填した。改質用触媒としては、ニッケルを約20重量%担持した平均粒径3mmのアルミナ粒子を用いた。吸収材としては、リチウムシリケート粉末を加圧成形することにより直径5mm、長さ5mmとした圧粉体(多孔質体)を用いた。
再生工程の反応管内の温度を700℃にした以外、実施例1と同様な方法で改質および再生を100回繰返した。
再生工程での処理ガスとして二酸化炭素を5体積%含む窒素ガスを用い、反応管内の温度を650℃にした以外、実施例1と同様な方法で改質および再生を100回繰返した。
再生工程での窒素ガスの供給をエタノール水溶液の蒸気と同じ、上から下に向けるダウンフローで行った以外、実施例1と同様な方法で改質および再生を100回繰返した。
再生工程の反応管内の温度を600℃にした以外、実施例1と同様な方法で改質および再生を100回繰返した。
Claims (3)
- 原料ガスおよび水蒸気を導入するためのガス導入部および改質反応ガスの排出部を有する改質器内に改質用触媒とリチウムシリケートを含む二酸化炭素を吸収するための吸収材とを充填し、原料ガスおよび水蒸気を前記ガス導入部を通して改質器内に供給して水蒸気改質反応を行い、水素と同時に副生した二酸化炭素を前記吸収材で吸収し、その吸収材による二酸化炭素の吸収能力が低下した後、前記吸収材から二酸化炭素を放出させて吸収材を再生する方法であって、
前記改質器内の温度を625℃以上に設定し、かつ不活性ガスまたは二酸化炭素を5体積%以下含む不活性ガスを処理ガスとして前記改質器内に前記原料ガスおよび水蒸気の供給方向と向きが反対になるよう前記排出部を通して供給することを特徴とする吸収材の再生方法。 - 前記原料ガスがエタノールを主成分とすることを特徴とする請求項1記載の吸収材の再生方法。
- 前記改質器内の温度の上限が720℃であることを特徴とする請求項1または2記載の吸収材の再生方法。
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