Photoinitiated Energy Transfer in Porous‐Cage‐Stabilised Silver Nanoparticles

Wilms, Michael; Melendez, Lesly V.; Hudson, Rohan J.; Ratnayake, Samantha Prabath; Smith, Trevor A.; Gaspera, Enrico Della; Bryant, Gary; Connell, Timothy U.; Gómez, Daniel E.

doi:10.1002/anie.202303501

Cited by 3 publications

(2 citation statements)

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“…Molecular cages are three-dimensional molecules with well-defined internal cavities. , The design of intricate supramolecular capsules, initially driven by their unique structures and aesthetic appeal, led to the discovery of their remarkable properties and functions, stimulating developments in supramolecular chemistry. Metal–organic capsules demonstrate numerous intriguing features that allow their exploitation in separating small molecules, sensing, metal nanoparticle generation, drug delivery, and anion transport . The tailored voids of molecular capsules, protected from the surrounding, allow entrapment of reactive species which was exploited to perform catalytic transformations that would be unattainable under typical reaction conditions .…”

Section: Introductionmentioning

confidence: 99%

Argentophilic Interactions, Flexibility, and Dynamics of Pyrrole Cages Encapsulating Silver(I) Clusters

Trzaskowski,

Martínez,

Sarwa

et al. 2024

J. Phys. Chem. A

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Recently, pyrrole cages have been synthesized that encapsulate ion pairs and silver(I) clusters to form intricate supramolecular capsules. We report here a computational analysis of these structures using density functional theory combined with a semiempirical tight-binding approach. We find that for neutral pyrrole cages, the Gibbs free energies of formation provide reliable predictions for the ratio of bound ions. For charged pyrrole cages, we find strong argentophilic interactions between Ag ions on the basis of the calculated bond indices and molecular orbitals. For the cage with the Ag 4 cluster, we find two minimum-geometry conformations that differ by only 6.5 kcal/mol, with an energy barrier <1 kcal/mol, suggesting a very flexible structure as indicated by molecular dynamics. The predicted energies of formation of [Ag n ⊂1] n-3+ (n = 1−5) cryptands provide low energy barriers of formation of 5−20 kcal/mol for all cases, which is consistent with the experimental data. Furthermore, we also examined the structural variability of mixed-valence silver clusters to test whether additional geometrical conformations inside the organic cage are thermodynamically accessible. In this context, we show that the time-dependent density functional theory UV−vis spectra may potentially serve as a diagnostic probe to characterize mixed-valence and geometrical configurations of silver clusters encapsulated into cryptands.

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Section: Introductionmentioning

confidence: 99%

Argentophilic Interactions, Flexibility, and Dynamics of Pyrrole Cages Encapsulating Silver(I) Clusters

Trzaskowski,

Martínez,

Sarwa

et al. 2024

J. Phys. Chem. A

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“…In previous works, enormous attention has been developed for producing Ag NPs’ carriers, and a wide variety of carrier materials have emerged, including silica, graphene oxide (GO), , porous carbon materials, , and organic/inorganic polymeric micro/nanoparticles . In one study, You et al successfully prepared Ag NPs on the surface of negatively charged alginate microspheres for the catalytic reduction of 4-nitrophenol.…”

Section: Introductionmentioning

confidence: 99%

Tannin-Assisted Synthesis of Nanocomposites Loaded with Silver Nanoparticles and Their Multifunctional Applications

Xia,

Jiang,

et al. 2023

Biomacromolecules

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Nanocomposites have been widely used in many important areas due to their particular physical/chemical properties; however, just though a simple technology, endowing multiple functions into a single nanomaterial for realizing their multifunctional applications is still a challenge. Here, we report a robust method for the facile synthesis of Ag-based multifunctional nanocomposites via using tannin-coated phenol–formaldehyde resin nanospheres (TA-PFRN) as silver nanoparticle (Ag NP) carriers. The thickness of the tannin coating is readily tuned from 50 to 320 nm by regulating the concentration of tannin added. Under the optimal conditions, the TA-PFRN has a 23.8 wt % of Ag NPs loading capacity with only 17.2 nm Ag NP layers. Consequently, the novel TA-PFRN@Ag nanocomposites possess multiple functions and integrated characteristics. As catalysts, the catalytic efficiency of TA-PFRN@Ag is nearly 6 times higher than that of the PFRN@Ag. As highly effective free radical initiators, TA-PFRN@Ag nanocomposites can trigger ultrafast acrylic acid (AA)/acrylamide (AM) polymerization at room temperature (in only a few minutes). As nano-reinforced fillers, the addition of 0.04 wt % nanocomposites can improve the tensile strength of PVA film from 60 to 153.2 MPa. In addition, the nanocomposites can also serve as antibacterial agents, efficiently inhibiting the growth of Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus); as antiultraviolet agents, the presence of TA-PFRN@Ag nanocomposites endows the film/hydrogel materials excellent ultraviolet (UV) shielding. This work provides a novel strategy for the green synthesis of Ag-based multifunctional nanocomposites that show promising applications in catalysis, nanomaterials, and biomedicine.

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