2020
DOI: 10.1002/anie.201916578
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Highly Mesoporous Metal‐Organic Frameworks as Synergistic Multimodal Catalytic Platforms for Divergent Cascade Reactions

Abstract: 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 sing… Show more

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Cited by 87 publications
(65 citation statements)
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“…However, a study published in early 2020 provides an example of a MOFbased MCHM featuring enzymes incorporated within the material pores. 44 This breakthrough was achieved through the use of polyvinylpyrrolidone (PVP), a non-ionic amphiphilic polymer, for the generation of mesopores (>20 nm) during the crystallisation of a MOF based on the structure of cobaltcontaining zeolite imidazolates (ZIF-67). PVP was used as a bulky polymer that participated in metal coordination during the crystallisation of ZIF-67 and thus partially disrupted the catenation of the imidazole-Co(II) complex to afford a crystal structure with abundant mesopores, more commonly referred to as holes.…”
Section: Use Of Flexible Supportsmentioning
confidence: 99%
“…However, a study published in early 2020 provides an example of a MOFbased MCHM featuring enzymes incorporated within the material pores. 44 This breakthrough was achieved through the use of polyvinylpyrrolidone (PVP), a non-ionic amphiphilic polymer, for the generation of mesopores (>20 nm) during the crystallisation of a MOF based on the structure of cobaltcontaining zeolite imidazolates (ZIF-67). PVP was used as a bulky polymer that participated in metal coordination during the crystallisation of ZIF-67 and thus partially disrupted the catenation of the imidazole-Co(II) complex to afford a crystal structure with abundant mesopores, more commonly referred to as holes.…”
Section: Use Of Flexible Supportsmentioning
confidence: 99%
“…Cascade reactions enable two or more steps in a one-pot reaction without isolation of intermediates to bypass tedious workups, degradation of the intermediates, and the cost and time associated with pharmaceutical and chemical manufacturing. [1][2] In particular, chemo-enzymatic cascade reactions represent an emerging strategy in chemical synthesis, and enable novel synthetic pathways that combine the reactivity of chemical catalysts with the selectivity of enzymes, create useful one-pot transformations unattainable with biocatalysts or chemocatalysts alone. 1,[3][4] However, the major challenges that need to be addressed are still the compatibility problems and mutual inactivation upon combining chemocatalysts with biocatalysts.…”
Section: Introductionmentioning
confidence: 99%
“…1,[3][4] However, the major challenges that need to be addressed are still the compatibility problems and mutual inactivation upon combining chemocatalysts with biocatalysts. [1][2]5 By far, a majority of the current reported strategies relied on homogeneous reactions where toxic co-solvents and phase-transferable reagents were routinely used to increase compatibility. [6][7][8] A biphasic reaction offers several advantages over a homogeneous reaction, such as environment-friendly processes, easy isolation, and separation of the catalyst from the reaction mixture, thus reducing downstream costs.…”
Section: Introductionmentioning
confidence: 99%
“…23 However, with the nanoreactors developed so far, the enzyme is encapsulated in or on a carrier, and the shell of the nanoreactor shell constitutes an additional diffusion barrier slowing down the influx rate of reactants. 24 In such case, complex membrane modifications are required to ensure the nanoreactor permeability. 19,25 Furthermore, the use of any additional carrier material, such as lipids or polymers, limits the effective enzyme concentration in the system due to the volume occupied by the non-catalytic carrier.…”
Section: Introductionmentioning
confidence: 99%