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Supramolecular regulation of bioorthogonal catalysis in cells using nanoparticle-embedded transition metal catalysts.


ABSTRACT: Bioorthogonal catalysis broadens the functional possibilities of intracellular chemistry. Effective delivery and regulation of synthetic catalytic systems in cells are challenging due to the complex intracellular environment and catalyst instability. Here, we report the fabrication of protein-sized bioorthogonal nanozymes through the encapsulation of hydrophobic transition metal catalysts into the monolayer of water-soluble gold nanoparticles. The activity of these catalysts can be reversibly controlled by binding a supramolecular cucurbit[7]uril 'gate-keeper' onto the monolayer surface, providing a biomimetic control mechanism that mimics the allosteric regulation of enzymes. The potential of this gated nanozyme for use in imaging and therapeutic applications was demonstrated through triggered cleavage of allylcarbamates for pro-fluorophore activation and propargyl groups for prodrug activation inside living cells.

SUBMITTER: Tonga GY 

PROVIDER: S-EPMC5697749 | biostudies-literature | 2015 Jul

REPOSITORIES: biostudies-literature

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Supramolecular regulation of bioorthogonal catalysis in cells using nanoparticle-embedded transition metal catalysts.

Tonga Gulen Yesilbag GY   Jeong Youngdo Y   Duncan Bradley B   Mizuhara Tsukasa T   Mout Rubul R   Das Riddha R   Kim Sung Tae ST   Yeh Yi-Cheun YC   Yan Bo B   Hou Singyuk S   Rotello Vincent M VM  

Nature chemistry 20150701 7


Bioorthogonal catalysis broadens the functional possibilities of intracellular chemistry. Effective delivery and regulation of synthetic catalytic systems in cells are challenging due to the complex intracellular environment and catalyst instability. Here, we report the fabrication of protein-sized bioorthogonal nanozymes through the encapsulation of hydrophobic transition metal catalysts into the monolayer of water-soluble gold nanoparticles. The activity of these catalysts can be reversibly co  ...[more]

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