Systematic construction of progressively larger capsules from a fivefold linking pyrrole-based subcomponent

Kai, Wu; Ronson, Tanya K.; Su, Pingru; Chen, Zhi; Goh, Leonard; Heard, Andrew W.; Li, Xiaopeng; Klautzsch, Fabian; Schalley, Christoph A.; Vinković, Mladen; Nitschke, Jonathan R.

doi:10.1038/s44160-023-00276-9

Cited by 18 publications

(19 citation statements)

References 36 publications

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“…A 1 H diffusion-ordered spectroscopy (DOSY) experiment indicated the formation of a single species, with a diffusion coefficient ( D ) of 2.19 × 10 –10 m 2 s –1 , corresponding to a solvodynamic radius of 2.7 nm (Figures b, S11 and S12). The results are in line with the expected size of Zn-1 , consistent with the crystal structure of a previously described Co II analog . Electrospray ionization mass spectrometry (ESI-MS) further confirmed its Zn II 20 L 12 composition, while traveling wave ion mobility-mass spectrometry (TWIM-MS) data excluded the presence of other isomers (Figure d,e).…”

Section: Resultssupporting

confidence: 89%

“…21 The results are in line with the expected size of Zn-1, consistent with the crystal structure of a previously described Co II analog. 18 Electrospray ionization mass spectrometry (ESI-MS) further confirmed its Zn II 20 L 12 composition, while traveling wave ion mobility-mass spec-trometry (TWIM-MS) data excluded the presence of other isomers (Figure 2d,e). Small-angle X-ray scattering (SAXS) analysis offers a statistically robust method for the structural characterization of large cages.…”

Section: ■ Results and Discussionmentioning

confidence: 92%

“…Different stimuli, such as the addition of subcomponents, metal ions, or a change in temperature, triggered the transformation of one cage into another. The use of graph theory to extend our original series of truncated polyhedra 18 allowed us to characterize a new pseudo-truncated octahedral structure, which crystallized with either D 4 , D 2 , or C 2 symmetry. In contrast to the structural diversity we obtained previously, 18 here a complex transformation network between four large cages and one sandwich structure was realized, with different stimuli triggering structural interconversions.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…A distinct strategy was previously developed to construct a series of progressively larger capsules with formulas of M 5n L 2n , where n = 1, 2, 3, or 6, by increasing the dihedral angles between pentagonal faces at vertices. 18 We reasoned that M 5n L 2n structures with values of n missing from this series might be obtained by modifying the angles between the pentagonal faces of these structures. Based on graph theory 23 we proposed a structure for the Zn II 20 L 8 cage (n = 4, Figure S1), having a measured angle of ∼90°.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…We infer the structure of Zn-3 to have the same truncated rhombohedral framework as a reported truncated rhombohedron with Co II centers. 18 Tetrabutylammonium G could not be removed even by washing with diethyl ether three times, highlighting the strong interactions between host and guest, which might lead to the cage transformation as discussed below. This truncated rhombohedral structure possesses eight triangular windows and three edge window pockets, where two pentagonal faces share the same edge.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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A Diverse Array of Large Capsules Transform in Response to Stimuli

et al. 2023

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The allosteric regulation of biomolecules, such as enzymes, enables them to adapt and alter their conformation to fit specific substrates, expressing different functionalities in response to stimuli. Different stimuli can also trigger synthetic coordination cages to change their shape, size, and nuclearity by reconfiguring the dynamic metal−ligand bonds that hold them together. Here we demonstrate an abiological system consisting of different organic subcomponents and Zn II metal ions, which can respond to simple stimuli in complex ways. A Zn II 20 L 12 dodecahedron transforms to give a larger Zn II 30 L 12 icosidodecahedron through subcomponent exchange, as an aldehyde that forms bidentate ligands is displaced in favor of one that forms tridentate ligands together with a pentaamine subcomponent. In the presence of a chiral template guest, the same system that produced the icosidodecahedron instead gives a Zn II 15 L 6 truncated rhombohedral architecture through enantioselective self-assembly. Under specific crystallization conditions, a guest induces a further reconfiguration of either the Zn II 30 L 12 or Zn II 15 L 6 cages to yield an unprecedented Zn II 20 L 8 pseudo-truncated octahedral structure. The transformation network of these cages shows how large synthetic hosts can undergo structural adaptation through the application of chemical stimuli, opening pathways to broader applications.

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Section: Resultssupporting

confidence: 89%

Section: ■ Results and Discussionmentioning

confidence: 92%

Section: ■ Results and Discussionmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

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A Diverse Array of Large Capsules Transform in Response to Stimuli

et al. 2023

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Microenvironment‐Adaptive Metallo‐Polymeric Nanodecoys via Subcomponent Coordination for Bacterial Biofilm Eradication and Immunomodulation

Li,

Hua,

et al. 2024

Adv Funct Materials

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Biofilm‐associated infections pose complex challenges that require addressing the multifaceted requirements of biofilm disruption, bacterial killing, and immunomodulation. In this study, microenvironment‐adaptive metallo‐polymeric nanodecoys (MPNs) are synthesized through one‐pot subcomponent coordination in aqueous solution, effectively eradicating bacterial biofilms and modulating immune response. Within the acidic microenvironment of biofilms, the positively charged MPNs demonstrated the ability to interact with and eliminate bacteria while facilitating a Fenton‐like reaction for efficient eradication of bacterial biofilms. As the local microenvironment shifted from a neutral to a basic state during subsequent tissue healing processes, the MPNs adaptively harness the multiple properties to bind pathogen‐associated molecular patterns, scavenge reactive oxygen species, thereby modulating the immune response, alleviating inflammation, and promoting tissue healing. This study presents an efficient strategy for preparing enzyme‐mimicking materials that closely resemble natural metalloenzymes, and the MPNs offer an efficient alternative to current antibiotic treatments for biofilm‐associated infections.

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Photoluminescent Cu(I) Assemblies with High‐Temperature Solid‐State Transitions as a New Class of Thermic History Tracers

Schlachter,

Moutier,

Utrera‐Melero

et al. 2024

Advanced Optical Materials

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The preparation of a new series of luminescent one dimensional coordination polymers based on the association of a photoactive tetrametallic metallacycle Cu(I) precursor with pyridyl‐caped ditopic linkers is reported. In spite of related molecular architectures, these coordination polymers present upon Ultraviolet visible light photoexcitation markedly contrasted solid‐state luminescence behaviors including eye‐perceived colors of the emitted light spanning all over the visible spectrum. Solid‐state temperature‐dependent photophysical measurements and Time‐dependent density‐functional theory calculations have been conducted to identify the relaxation pathways lying in these assemblies. Very importantly, thermal stability studies at high temperature for all these derivatives reveal an irreversible post‐synthetic solid‐state transition that impacts dramatically the photophysical properties of these newly obtained phases, highlighting an innovative family of stimuli‐sensitive materials that can witness the exceeding of critical temperatures in their environment.

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Systematic construction of progressively larger capsules from a fivefold linking pyrrole-based subcomponent

Cited by 18 publications

References 36 publications

A Diverse Array of Large Capsules Transform in Response to Stimuli

A Diverse Array of Large Capsules Transform in Response to Stimuli

Microenvironment‐Adaptive Metallo‐Polymeric Nanodecoys via Subcomponent Coordination for Bacterial Biofilm Eradication and Immunomodulation

Photoluminescent Cu(I) Assemblies with High‐Temperature Solid‐State Transitions as a New Class of Thermic History Tracers

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