Amphiphilic polymeric nanoparticles enable homogenous rhodium-catalysed NH insertion reactions in living cells

Sathyan, Anjana; Loman, Tessa; Deng, Linlin; Palmans, Anja R. A.

doi:10.1039/d3nr02581k

Cited by 6 publications

(4 citation statements)

References 62 publications

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“…All solvents were purchased from Biosolve. The following polymers and compounds were synthesized according to previously developed protocols: pPFPA 180 [39], BTA amine [31], Gly 1, diyne 2, pro-rho 8, rho 9, 12-azidododecan-1-amine, and P4 [12,26,29,40].…”

Section: Materials and Instrumentsmentioning

confidence: 99%

Effect of Particle Heterogeneity in Catalytic Copper-Containing Single-Chain Polymeric Nanoparticles Revealed by Single-Particle Kinetics

Sathyan,

Archontakis,

Spiering

et al. 2024

Molecules

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Single-chain polymeric nanoparticles (SCPNs) have been extensively explored as a synthetic alternative to enzymes for catalytic applications. However, the inherent structural heterogeneity of SCPNs, arising from the dispersity of the polymer backbone and stochastic incorporation of different monomers as well as catalytic moieties, is expected to lead to variations in catalytic activity between individual particles. To understand the effect of structural heterogeneities on the catalytic performance of SCPNs, techniques are required that permit researchers to directly monitor SCPN activity at the single-polymer level. In this study, we introduce the use of single-molecule fluorescence microscopy to study the kinetics of Cu(I)-containing SCPNs towards depropargylation reactions. We developed Cu(I)-containing SCPNs that exhibit fast kinetics towards depropargylation and Cu-catalyzed azide-alkyne click reactions, making them suitable for single-particle kinetic studies. SCPNs were then immobilized on the surface of glass coverslips and the catalytic reactions were monitored at a single-particle level using total internal reflection fluorescence (TIRF) microscopy. Our studies revealed the interparticle turnover dispersity for Cu(I)-catalyzed depropargylations. In the future, our approach can be extended to different polymer designs which can give insights into the intrinsic heterogeneity of SCPN catalysis and can further aid in the rational development of SCPN-based catalysts.

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Section: Materials and Instrumentsmentioning

confidence: 99%

Effect of Particle Heterogeneity in Catalytic Copper-Containing Single-Chain Polymeric Nanoparticles Revealed by Single-Particle Kinetics

Sathyan,

Archontakis,

Spiering

et al. 2024

Molecules

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“…[68] Sathyan et al generated polymer nanoparticles comprising dodecyl and Jeffamine pendant groups and used these to encapsulate dirhodium II carboxylate complexes via chain collapse in water and matching of the polarity of suitable complexes to their hydrophobic interior. [87] Complexes with hydrophobic ligands were incorporated with efficiencies greater than 97 %, while a hydrophilic ligand complex was only incorporated with 50 % efficiency. As discussed above, the formed particles consisted of polymer chain aggregates, indicated by a size increase in DLS, hence not termed SCNP, but "amphiphilic polymer nanoparticles".…”

Section: Current State Of the Art In Scnp Catalysismentioning

confidence: 99%

Single Chain Nanoparticles in Catalysis

Mundsinger,

Izuagbe,

Tuten

et al. 2023

Angew Chem Int Ed

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Over the last six decades folded polymer chains – so‐called Single Chain Nanoparticles (SCNPs) – have evolved from the mere concept of intramolecularly crosslinked polymer chains to tailored nanoreactors, underpinned by a plethora of techniques and chemistries to tailor and analyze their morphology and function. These monomolecular polymer entities hold critical promise in a wide range of applications. Herein, we highlight the exciting progress that has been made in the field of catalytically active SCNPs within recent years.

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“…Im Jahr 2023 stellten Sathyan et al Polymernanopartikel her, die aus Dodecyl-und Jeffamine-Seitengruppen bestanden, um Dirhodium(II)-Carboxylatkomplexe, deren Polarität an den hydrophoben Partikelkern angepasst wurde, durch Kettenfaltung in Wasser einzuschließen. [87] Komplexe mit hydrophoben Liganden wurden mit Wirkungsgraden von mehr als 97 % und ein Komplex mit hydrophilen Liganden nur mit 50 % Effizienz eingeschlossen. Wie bereits diskutiert, bestanden die Partikel aus Aggregaten von Polymerketten, welche durch eine Größenzunahme mittels DLS nachgewiesen, wurden.…”

Section: Stand Der Technik In Der Eknp Katalyseunclassified

Einzelkettennanopartikel in der Katalyse

Mundsinger,

Izuagbe,

Tuten

et al. 2023

Angewandte Chemie

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Amphiphilic polymeric nanoparticles enable homogenous rhodium-catalysed NH insertion reactions in living cells

Abstract: Hydrophobic dirhodium complexes embedded into amphiphilic nanoparticles catalyse efficiently the in vitro formation of fluorescent and cytotoxic quinoxalines.

Cited by 6 publications

References 62 publications

Effect of Particle Heterogeneity in Catalytic Copper-Containing Single-Chain Polymeric Nanoparticles Revealed by Single-Particle Kinetics

Effect of Particle Heterogeneity in Catalytic Copper-Containing Single-Chain Polymeric Nanoparticles Revealed by Single-Particle Kinetics

Single Chain Nanoparticles in Catalysis

Einzelkettennanopartikel in der Katalyse

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