Highly Mesoporous Metal‐Organic Frameworks as Synergistic Multimodal Catalytic Platforms for Divergent Cascade Reactions

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  • Soumen Dutta
    Center for Nanospace-confined Chemical Reactions (NCCR) Pohang University of Science and Technology (POSTECH) Pohang 37673 South Korea
  • Nitee Kumari
    Center for Nanospace-confined Chemical Reactions (NCCR) Pohang University of Science and Technology (POSTECH) Pohang 37673 South Korea
  • Sateesh Dubbu
    Center for Nanospace-confined Chemical Reactions (NCCR) Pohang University of Science and Technology (POSTECH) Pohang 37673 South Korea
  • Sun Woo Jang
    Center for Nanospace-confined Chemical Reactions (NCCR) Pohang University of Science and Technology (POSTECH) Pohang 37673 South Korea
  • Amit Kumar
    Center for Nanospace-confined Chemical Reactions (NCCR) Pohang University of Science and Technology (POSTECH) Pohang 37673 South Korea
  • Hiroyoshi Ohtsu
    Department of Chemistry School of Science Tokyo Institute of Technology Tokyo 152-8550 Japan
  • Junghoon Kim
    Department of Chemistry Pohang University of Science and Technology (POSTECH) Pohang 37673 South Korea
  • Seung Hwan Cho
    Department of Chemistry Pohang University of Science and Technology (POSTECH) Pohang 37673 South Korea
  • Masaki Kawano
    Department of Chemistry School of Science Tokyo Institute of Technology Tokyo 152-8550 Japan
  • In Su Lee
    Center for Nanospace-confined Chemical Reactions (NCCR) Pohang University of Science and Technology (POSTECH) Pohang 37673 South Korea

書誌事項

公開日
2020-02-03
資源種別
journal article
権利情報
  • http://onlinelibrary.wiley.com/termsAndConditions#vor
DOI
  • 10.1002/anie.201916578
  • 10.1002/ange.201916578
公開者
Wiley

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説明

<jats:title>Abstract</jats:title><jats:p>Rational engineering and assimilation of diverse chemo‐ and biocatalytic functionalities in a single nanostructure is highly desired for efficient multistep chemical reactions but has so far remained elusive. Here, we design and synthesize multimodal catalytic nanoreactors (MCNRs) based on a mesoporous metal‐organic framework (MOF). The MCNRs consist of customizable metal nanocrystals and stably anchored enzymes in the mesopores, as well as coordinatively unsaturated cationic metal MOF nodes, all within a single nanoreactor space. The highly intimate and diverse catalytic mesoporous microenvironments and facile accessibility to the active site in the MCNR enables the cooperative and synergistic participation from different chemo‐ and biocatalytic components. This was shown by one‐pot multistep cascade reactions involving a heterogeneous catalytic nitroaldol reaction followed by a [Pd/lipase]‐catalyzed chemoenzymatic dynamic kinetic resolution to yield optically pure (>99 % ee) nitroalcohol derivatives in quantitative yields.</jats:p>

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