JP2020028881A - 分離膜構造体及びガスの分離方法 - Google Patents
分離膜構造体及びガスの分離方法 Download PDFInfo
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- JP2020028881A JP2020028881A JP2019208517A JP2019208517A JP2020028881A JP 2020028881 A JP2020028881 A JP 2020028881A JP 2019208517 A JP2019208517 A JP 2019208517A JP 2019208517 A JP2019208517 A JP 2019208517A JP 2020028881 A JP2020028881 A JP 2020028881A
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- Prior art keywords
- separation membrane
- nitrogen
- membrane
- separation
- pore diameter
- Prior art date
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Classifications
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Abstract
Description
図1は、分離膜構造体10の構成を示す断面図である。分離膜構造体10は、少なくともメタン分子(以下、「メタン」と略称する。)と窒素分子(以下、「窒素」と略称する。)を含有する混合ガス中の窒素を選択的に透過させる。分離膜構造体10は、多孔質支持体20、第1分離膜30及び第2分離膜40を備える。
分離膜構造体10の製造方法について説明する。
まず、押出成形法、プレス成形法あるいは鋳込み成形法などを用いて、基体21の原料を所望の形状に成形することによって基体21の成形体を形成する。次に、基体21の成形体を焼成(例えば、900℃〜1450℃)して基体21を形成する。
多孔質支持体20の表面に第1分離膜30を形成する。第1分離膜30は、膜種に応じた従来既知の手法で形成することができる。以下、第1分離膜30の形成手法の一例としてゼオライト膜、シリカ膜及び炭素膜それぞれの形成方法を順次説明する。
まず、種結晶としてのゼオライトを予め表層23の表面に塗布した後、シリカ源、アルミナ源、有機テンプレート、アルカリ源及び水などを含む原料溶液が入った耐圧容器に多孔質支持体20を浸漬する。
まず、テトラエトシキシランなどのアルコキシシラン、メチルトリメトキシシランなどの有機アルコキシシラン、又はカルボキシエチルシラントリオールナトリウム塩などの有機ヒドロキシシランを硝酸や塩酸等の触媒の存在下で加水分解や縮合させてゾル液とし、エタノール又は水で希釈することによって前駆体溶液(シリカゾル液)を調製する。
まず、エポキシ樹脂やポリイミド樹脂などの熱硬化性樹脂、ポリエチレンなどの熱可塑性樹脂、セルロース系樹脂、又はこれらの前駆体物質を、メタノール、アセトン、テトラヒドロフラン、NMP、トルエン等の有機溶媒や水に溶解することによって前駆体溶液を調製する。
第1分離膜30の表面に第2分離膜40を形成する。第2分離膜40は、膜種に応じた従来既知の手法で形成することができる。従って、第1分離膜30の形成手法に準じて第2分離膜40を形成できる。以下、ゼオライト膜、シリカ膜及び炭素膜の形成方法を順次説明する。
まず、種結晶としてのゼオライトを予め第1分離膜30の表面に塗布した後、シリカ源、アルミナ源、有機テンプレート、アルカリ源及び水に窒素吸着性金属カチオン及び窒素吸着性金属錯体の少なくとも一方が添加された原料溶液の入った耐圧容器に多孔質支持体20を浸漬する。この際、窒素吸着性金属カチオンや窒素吸着性金属錯体の添加量を調整することによって、第2分離膜40の窒素吸着性を制御することができる。なお、種結晶の塗布は行わなくてもよい。
まず、テトラエトシキシランなどのアルコキシシラン、メチルトリメトキシシランなどの有機アルコキシシラン、又はカルボキシエチルシラントリオールナトリウム塩などの有機ヒドロキシシランを硝酸の存在下で加水分解や縮合させてゾル液とし、窒素吸着性金属カチオン及び窒素吸着性金属錯体の少なくとも一方が添加されたエタノール又は水で希釈することによって前駆体溶液(シリカゾル液)を調製する。この際、窒素吸着性金属カチオンの添加量を調整することによって、第2分離膜40の窒素吸着性を制御することができる。
まず、エポキシ樹脂やポリイミド樹脂などの熱硬化性樹脂、ポリエチレンなどの熱可塑性樹脂、セルロース系樹脂、又はこれらの前駆体物質を、窒素吸着性金属カチオン及び窒素吸着性金属錯体の少なくとも一方が添加されたメタノール、アセトン、テトラヒドロフラン、NMP、トルエン等の有機溶媒や水に溶解することによって前駆体溶液を調製する。この際、窒素吸着性金属カチオンの添加量を調整することによって、第2分離膜40の窒素吸着性を制御することができる。
本実施形態に係る分離膜構造体10は、多孔質支持体20と、多孔質支持体20上に形成された第1分離膜30と、第1分離膜30上に形成された第2分離膜40とを備える。第1分離膜30は、0.32nm以上かつ0.44nm以下の平均細孔径を有する。第2分離膜40には、メタンに比べて窒素を吸着しやすい金属カチオン及び金属錯体の少なくとも一方が添加されている。
以上、本発明の一実施形態について説明したが、本発明は上記実施形態に限定されるものではなく、発明の要旨を逸脱しない範囲で種々の変更が可能である。
以下のようにして、サンプルNo.1に係る分離膜構造体を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
まず、サンプルNo.1と同じ多孔質アルミナ基材を作製した。
サンプルNo.1〜15に係る分離膜構造体を用いてガス分離試験を行った。
また、第2分離膜が同じサンプルNo.5〜8、11〜13のうち、変動係数が0.4以下であるサンプルNo.5〜8、11、12では窒素分離性能をより向上させることができた。
20 多孔質支持体
21 基体
22 中間層
23 表層
30 第1分離膜
40 第2分離膜
Claims (9)
- 少なくともメタンと窒素を含有する混合ガス中の窒素を選択的に透過させる分離膜構造体であって、
多孔質支持体と、
前記多孔質支持体上に形成され、0.32nm以上かつ0.44nm以下の平均細孔径を有する第1分離膜と、
前記第1分離膜上に形成され、金属カチオンが添加された第2分離膜と、
を備える分離膜構造体。 - 少なくともメタンと窒素を含有する混合ガス中の窒素を選択的に透過させる分離膜構造体であって、
多孔質支持体と、
前記多孔質支持体上に形成され、0.32nm以上かつ0.44nm以下の平均細孔径を有する第1分離膜と、
前記第1分離膜上に形成され、Si/Al比が第1分離膜より低い第2分離膜と、
を備え、
前記第1分離膜及び前記第2分離膜それぞれは、ゼオライトによって構成される、
分離膜構造体。 - 前記第2分離膜の平均細孔径は、前記第1分離膜の平均細孔径以上である、
請求項1又は2に記載の分離膜構造体。 - 前記第2分離膜の平均細孔径は、前記第1分離膜の平均細孔径よりも大きい、
請求項1又は2に記載の分離膜構造体。 - 前記第2分離膜に添加される前記金属カチオンは、Sr、Mg、Li、Ba、Ca、Cu、Feから選択される少なくとも1種である、
請求項1に記載の分離膜構造体。 - 前記第2分離膜に添加される前記金属カチオンの総濃度は、0.01%以上60%以下である、
請求項1に記載の分離膜構造体。 - 前記第2分離膜に添加される前記金属カチオンの総濃度は、0.03%以上50%以下である、
請求項1に記載の分離膜構造体。 - 前記第1分離膜の細孔径の標準偏差を前記平均細孔径で割った変動係数は、0.4以下である、
請求項1乃至7のいずれかに記載の分離膜構造体。 - 請求項1乃至8のいずれかに記載の分離膜構造体を用いて、少なくともメタンと窒素を含有する混合ガス中の窒素を選択的に透過させる、
ガスの分離方法。
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