JP7335868B2 - ジアミン付加金属有機骨格における2ステップ二酸化炭素吸着の克服 - Google Patents
ジアミン付加金属有機骨格における2ステップ二酸化炭素吸着の克服 Download PDFInfo
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Description
近時、図1aに図示したMg2+部位で裏打ちされた1次元の六角形チャネルを有する金属有機骨格であるMg2(dobpdc)(dobpdc4-=4,4’-ジオキシビフェニル-3,3’-ジカルボキシレート)の開いたMg2+部位に対してアルキルエチレンジアミンおよびアルキルプロピレンジアミンを合成後に付加させることにより調製されるジアミン付加金属有機骨格の新しいクラスが評価されている。McDonald et al.,2015,Nature 519,p.303、Drisdell et al.,2015,Phys Chem Chem Phys 17,p.2144、McDonald,2012,J.Am.Chem.Soc.134,p.7056、Jo et al.,2017,ChemSusChem 10,p.541、Lee et al.,2015,Chem.Sci.6,p.3697、およびLee et al.2014,Energy Environ.Sci.7,p.744を参照されたい。ジアミンを官能化すると(図1b)、これらの材料は、付加されたジアミンの構造を制御することによって調整され得るステップ圧力で、CO2のステップ状吸着を示す。これらのS字状の吸着プロファイルは、c軸に沿って高度に安定化されたカルバミン酸アンモニウム鎖(図1c)の協同形成から生じ、最小の温度スイング(例えば、ΔT=60℃)によって高い作業容量(>2.5mmol/g)を実現することができる。McDonald et al.,2015,Nature 519,p.303を参照されたい。さらに、これらの材料は、一般に、湿潤条件下でも、適度な再生エネルギーおよび高いCO2/N2選択性を備えている。Mg2(dobpdc)のジアミン付加変異体に関する分析により、e-2およびi-2などの1°,2°-アルキルエチレンジアミン(図1d)が、低いCO2吸着ステップ圧力(≦1mbar、40℃)と、二級、二級(2°,2°)ジアミンと比較したジアミン損失に対する安定性に起因して、希釈ガス流からのCCSに関して最も有望であることが示唆される。しかしながら、本開示の前に、これらのジアミン付加金属有機骨格が、CCSプロセスでの長期適用に求められる必須の安定性を有するかどうかは不明なままであった。
置換基が、左から右に書かれたそれらの従来の化学式によって特定される場合、その構造は、任意選択的に、右から左へ構造を書くことによって生じることになる化学的に同一の置換基も包含し、例えば、-CH2O-は、任意選択的に-OCH2-も列挙していることが意図される。
本開示の一態様は、吸着材料を提供する。吸着材料は、複数の金属イオンおよび複数のポリトピック有機リンカーを含む金属有機骨格を含む吸着材料を含み、複数のポリトピック有機リンカーにおける各ポリトピック有機リンカーは、複数の金属イオンにおける少なくとも2つの金属イオンに接続される。吸着材料は、複数の配位子をさらに含み、複数の配位子における各それぞれの配位子は、金属有機骨格の複数の金属イオン中の金属イオンにアミン付加されている。複数の配位子において各それぞれの配位子は、以下を含み、
いくつかの実施形態では、ポリトピック有機リンカーは、以下の式を有する:
本開示の一態様では、開示された吸着材料に関するいくつかの技術用途を提供する。
本明細書に記載した実施例および実施形態は、単に例示を目的とし、それを踏まえた様々な修正または変更が当業者に示唆され、本出願の趣旨および権限ならびに添付の特許請求の範囲内に含まれることが理解される。本明細書で引用したすべての刊行物、特許、および特許出願は、あらゆる目的のためにそれらの全体が参照により本明細書に組み込まれる。
Claims (16)
- 吸着材料であって、
複数の金属イオンおよび複数のポリトピック有機リンカーを含む金属有機骨格であって、前記複数のポリトピック有機リンカーにおける各ポリトピック有機リンカーが、前記複数の金属イオンにおける少なくとも2つの金属イオンに接続されている、金属有機骨格と、
複数の配位子であって、前記複数の配位子における各それぞれの配位子は、前記金属有機骨格の前記複数の金属イオンにおける金属イオンにアミン付加されており、前記複数の配位子における各それぞれの配位子が、以下を含む、
Xは、Mg、またはZnであり、
Zは、炭素であり、
Qは、炭素であり、
R1、R2、R3、R4、R5、R7、およびR8はそれぞれ独立して、H、ハロゲン、非置換もしくはハロゲン置換アルキル、非置換もしくはハロゲン置換ヘテロアルキル、非置換アリール、非置換もしくはハロゲン置換ヘテロアリール、または非置換ヘテロシクロアルキルから選択され、
R6は、少なくとも3個の非水素原子を含む、非置換もしくはハロゲン置換アルキル、非置換もしくはハロゲン置換ヘテロアルキル、非置換アリール、非置換もしくはハロゲン置換ヘテロアリール、または非置換ヘテロシクロアルキルである)複数の配位子と、を含み、
前記複数のポリトピック有機リンカーにおける各ポリトピック有機リンカーが、下式を有する、
吸着材料。 - R6が、3~10個の炭素原子を有する非置換アルキルである、請求項1に記載の吸着材料。
- R6が、3~10個の炭素原子を有するn-アルカンである、請求項1に記載の吸着材料。
- R6が、分枝鎖アルカン、非置換ヘテロシクロアルキル、または非置換シクロアルカンである、請求項1に記載の吸着材料。
- R6が、置換もしくは非置換シクロプロパン、シクロブタン、シクロペンタン、またはシクロヘキサンである、請求項1に記載の吸着材料。
- R1が、水素である、請求項1~5のいずれか一項に記載の吸着材料。
- 前記複数の金属イオンにおける各金属イオン(X)が、Mgである、請求項1~6のいずれか一項に記載の吸着材料。
- 前記複数の配位子における各配位子が、N-(n-ヘプチル)エチレンジアミンである、請求項1に記載の吸着材料。
- 前記ポリトピック有機リンカーが、3、3’-ジオキシドビフェニル-4,4’-ジカルボキシレート(パラ-カルボキシレート-dobpdc4-)である、請求項1、7、または8のいずれか一項に記載の吸着材料。
- 前記吸着材料が、少なくとも3050m2/gの77K N2ブルナウアー・エメット・テラー(BET)表面積を有する、請求項1に記載の吸着材料。
- 前記吸着材料が、少なくとも5800m2/gのラングミュア表面積を有する、請求項1に記載の吸着材料。
- 前記吸着材料の結晶学的密度が、0.4g/cm3~1.2g/cm3である、請求項1に記載の吸着材料。
- 前記複数の配位子における各それぞれの配位子が、以下を含み、
- 前記複数の配位子における各それぞれの配位子が、以下を含み、
- 供給源によって生成された二酸化炭素を隔離する方法であって、請求項1~14のいずれか一項に記載の吸着材料に前記二酸化炭素を曝露することと、それにより前記二酸化炭素が、前記吸着材料中に可逆的に隔離されることと、を含む、方法。
- 前記方法が、温度スイング吸着法、真空スイング吸着法、圧力スイング吸着法、濃度スイング吸着法、またはそれらの組み合わせを使用して、CO2に富む前記吸着材料を再生させることをさらに含む、請求項15に記載の方法。
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