Molecularly pure miktoarm spherical nucleic acids: preparation and usage as a scaffold for abiotic intracellular catalysis

Zhang, Bohan; Bai, Silei; Chao, Xiangyu; Wu, Tong; Chen, Zhiyong; Cheng, Zehong; Xiao, Yue; Zhang, Ke; Bai, Yugang

doi:10.1039/d1sc04833c

Cited by 6 publications

(1 citation statement)

References 47 publications

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“…For Cu-MAC IF catalysis, the incubation Cu concentration needed could be as low as 1 μM, while the reported Cu concentration for successful intracellular CuAAC using small molecular Cu-TTA analog was at the millimolar level ( 30 ). Therefore, it can be seen that despite MAC IF needs to face GSH and other coordinating molecules in the cytosol, the negatively charged phosphates on the cell membrane and those embedded membrane proteins might have provided sheltering for these catalysts ( 31 , 32 ). By incubating HeLa cells with FLip bearing FITC-labeled TTA-Cu II catalyst, we observed that the Cu-MACs immobilized via the LiFT process were able to stay on the cell membrane for an extended time period, showing a high extent of membrane staining even after 48 hours with well-preserved catalytic activity (fig.…”

Section: Resultsmentioning

confidence: 99%

Orientation-controlled membrane anchoring of bioorthogonal catalysts on live cells via liposome fusion–based transport

Chen

Xie

et al. 2023

Sci. Adv.

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An obstacle to conducting diverse bioorthogonal reactions in living systems is the sensitivity of artificial metal catalysts. It has been reported that artificial metallocatalysts can be assembled in “cleaner” environments in cells for stabilized performance, which is powerful but is limited by the prerequisite of using specific cells. We report here a strategy to establish membrane-anchored catalysts with precise spatial control via liposome fusion–based transport (MAC-LiFT), loading bioorthogonal catalytic complexes onto either or both sides of the membrane leaflets. We show that the inner face of the cytoplasmic membrane serves as a reliable shelter for metal centers, protecting the complexes from deactivation thus substantially lowering the amount of catalyst needed for effective intracellular catalysis. This MAC-LiFT approach makes it possible to establish catalyst-protective systems with exclusively exogenous agents in a wide array of mammalian cells, allowing convenient and wider use of diverse bioorthogonal reactions in live cellular systems.

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Section: Resultsmentioning

confidence: 99%

Orientation-controlled membrane anchoring of bioorthogonal catalysts on live cells via liposome fusion–based transport

Chen

Xie

et al. 2023

Sci. Adv.

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Chondroitin Sulfate‐Coated Heteroduplex‐Molecular Spherical Nucleic Acids

Laine,

Deshpande,

Tähtinen

et al. 2024

ChemBioChem

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Molecular Spherical Nucleic Acids (MSNAs) are atomically uniform dendritic nanostructures and potential delivery vehicles for oligonucleotides. The radial formulation combined with covalent conjugation may hide the oligonucleotide content and simultaneously enhance the role of appropriate conjugate groups on the outer sphere. The conjugate halo may be modulated to affect the delivery properties of the MSNAs. In the present study, [60]fullerene‐based molecular spherical nucleic acids, consisting of a 2’‐deoxyribonucleotide and a ribonucleotide sequence, were used as hybridization‐mediated carriers (’’DNA and RNA‐carriers’’) for an antisense oligonucleotide, suppressing Tau protein, (i.e. Tau‐ASO) and its conjugates with chondroitin sulfate tetrasaccharides (CS) with different sulfation patterns. The impact of the MSNA carriers, CS‐moieties on the conjugates and the CS‐decorations on the MSNAs on cellular uptake and ‐ activity (Tau‐suppression) of the Tau‐ASO was studied with hippocampal neurons in vitro. The formation and stability of these heteroduplex ASO‐MSNAs were evaluated by UV melting profile analysis, polyacrylamide gel electrophoresis (PAGE), dynamic light scattering (DLS) and size exclusion chromatography equipped with a multi angle light scattering detector (SEC‐MALS). The cellular uptake and ‐ activity were studied by confocal microscopy and Western blot analysis, respectively.

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From Structure to Application: The Evolutionary Trajectory of Spherical Nucleic Acids

Wang,

Han,

2024

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Since the proposal of the concept of spherical nucleic acids (SNAs) in 1996, numerous studies have focused on this topic and have achieved great advances. As a new delivery system for nucleic acids, SNAs have advantages over conventional deoxyribonucleic acid (DNA) nanostructures, including independence from transfection reagents, tolerance to nucleases, and lower immune reactions. The flexible structure of SNAs proves that various inorganic or organic materials can be used as the core, and different types of nucleic acids can be conjugated to realize diverse functions and achieve surprising and exciting outcomes. The special DNA nanostructures have been employed for immunomodulation, gene regulation, drug delivery, biosensing, and bioimaging. Despite the lack of rational design strategies, potential cytotoxicity, and structural defects of this technology, various successful examples demonstrate the bright and convincing future of SNAs in fields such as new materials, clinical practice, and pharmacy.

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Molecularly pure miktoarm spherical nucleic acids: preparation and usage as a scaffold for abiotic intracellular catalysis

Abstract: Biocompatible nano-constructs, with definite molecular structures and programmable subunits, can potentially be used as biocatalysts with modular functional moieties.

Cited by 6 publications

References 47 publications

Orientation-controlled membrane anchoring of bioorthogonal catalysts on live cells via liposome fusion–based transport

Orientation-controlled membrane anchoring of bioorthogonal catalysts on live cells via liposome fusion–based transport

Chondroitin Sulfate‐Coated Heteroduplex‐Molecular Spherical Nucleic Acids

From Structure to Application: The Evolutionary Trajectory of Spherical Nucleic Acids

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