タンドム触媒のためのゼオライト包装のPtナノ粒子
Hong Je Cho1, Doyoung Kim1, Jing Li2
1Department of Chemical and Biomolecular Engineering , University of Delaware , Newark , Delaware 19716 , United States.
Journal of the American Chemical Society
|September 25, 2018
まとめ
ゼオライト触媒の中にプラチナナノ粒子 (PtNP) を封じ込めると,タンデム反応が強化される. この新しいアプローチは,フルフラルとアセトンの変換を望ましいC8製品に導いて,ワンポット触媒プロセスの選択性を改善します.
科学分野:
- 異質な触媒
- ナノ材料科学
- ゼオライト化学
背景:
- 化学合成の効率化には 連続反応を単一段階のプロセスに統合することが重要です
- ゼオライトマトリクスは金属ナノ粒子をカプセル化するための有望なプラットフォームを提供し,制御された触媒環境を可能にします.
- 金属と酸の部位を含むタンデム反応は複雑で,しばしば望ましくない副産物につながります.
研究 の 目的:
- MFIゼオライト内にプラチナナノ粒子 (PtNP) をカチオンポリマー支援戦略を用いてカプセル化する方法を開発する.
- フルフラルとアセトンを含むタンデム反応の選択性に対する Pt NP 封じ込めの影響を調査する.
- マテリアルアーキテクチャを制御することによって,タンデムカタリシスにおける製品配布の操作を実証する.
主な方法:
- PtNPを封じ込んでいるMFIゼオライトの合成は,カチオンポリマー補助法を用いる.
- 異なった分子サイズの基板を用いた運動研究により,Pt NP封じ込め効率の量化 (>90%)
- フルフラルとアセトンのタンデムアルドール凝縮と水素化における触媒性能の評価
主要な成果:
- HZSM-5ゼオライト内のPtNPの90%以上の封じ込みを達成した.
- HZSM-5のゼオライト包装のPtNPは,フェルフラルとアセトンのタンデムアルドール凝縮と水素化を選択的に触媒化し,C8製品を87%生成した.
- HZSM-5の封じ込まないPtNPは主にフルフルールの水素化と脱炭素化をもたらした.
結論:
- PtNPをMFIゼオライト内に閉じ込め,触媒の選択性を高める.
- ゼオライトマトリックス内のPtと酸の場所の空間的配置は,アルドール凝縮と水素化を好み,タンデム反応経路を指示する.
- この研究は,カプセル化を通じて触媒材料の構造を調整することによって,タンデム反応製品の分布を制御する最初の証拠を示しています.
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