プロピンのイソメリゼーションと選択的水素化:原子層沈殿によって改変された金属有機フレームワークのスクリーニング
Ryan A Hackler, Riddhish Pandharkar1, Magali S Ferrandon
1Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota-Twin Cities, 207 Pleasant Street SE, Minneapolis, Minnesota 55455, United States.
Journal of the American Chemical Society
|November 17, 2020
まとめ
この研究では,プロピンの変換のための最良の金属酸化物クラスタを見つけるために,高通量スクリーニングを使用した. NU-1000 MOFのコバルトと亜鉛の組み合わせは,望ましい製品に対する高い活性と選択性を示した.
科学分野:
- 材料科学
- カタリシス
- ナノテクノロジー
背景:
- メタル・オーガニック・フレームワーク (MOF) は,触媒に調整可能な多孔構造を提供します.
- 原子層沈殿 (ALD) は,金属クラスターをMOFに正確に組み込むことを可能にします.
- プロパインの変換は 価値ある化学物質の生産に不可欠です
研究 の 目的:
- 様々な金属酸化物群を触媒性プロピネイソメリゼーションと水素化のためにスクリーニングする.
- 選択的なプロピネ変換のための最適の単金属および二金属クラスタを特定する.
- 反応選択性と安定性におけるクラスター組成の役割を調査する.
主な方法:
- 多様な金属酸化物クラスター (≥8原子) をALD経由でNU-1000MOFに組み込む.
- プロピンの反応のための合成MOF触媒の高通量スクリーニング.
- プロパディエンへのイソメリゼーションとプロピレンへの水素化の触媒活性分析
主要な成果:
- 銅 (Cu) とコバルト (Co) のクラスターはプロピネをプロピレンに水素化するために最も活発でした.
- コバルト-亜鉛 (Co-Zn) バイメタリッククラスターは,亜鉛 (Zn) とカドミウム (Cd) モノメタリッククラスターとともに,プロパディーネへのイソメリゼーションで最も活発であった.
- 単一の金属と比較して,NU-1000のコ-Znクラスタはプロパンとコクシングへの過剰水素化を減少させた.
結論:
- 小分子変容のための最適な金属クラスタを発見するのに高通量スクリーニングは有効です.
- MOF内の特定の金属組合せ (例えば,Co-Zn) は,触媒プロセスにおける選択性と安定性を高めることができます.
- 金属特有のメカニズムの理解は,イソメリゼーションと水素化のための効率的な触媒の設計の鍵です.
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