Dataset Information

Dynamic Covalent Self-Assembly of Chloride- and Ion-Pair-Templated Cryptates.

ABSTRACT: While supramolecular hosts capable of binding and transporting anions and ion pairs are now widely available, self-assembled architectures are still rare, even though they offer an inherent mechanism for the release of the guest ion(s). In this work, we report the dynamic covalent self-assembly of tripodal, urea-based anion cryptates that are held together by two orthoester bridgeheads. These hosts exhibit affinity for anions such as Cl^- , Br^- or I^- in the moderate range that is typically advantageous for applications in membrane transport. In unprecedented experiments, we were able to dissociate the Cs⋅Cl ion pair by simultaneously assembling suitably sized orthoester hosts around the Cs⁺ and the Cl^- ion.

SUBMITTER: Hollstein S

PROVIDER: S-EPMC9400851 | biostudies-literature | 2022 Jul

REPOSITORIES: biostudies-literature

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Publications

Dynamic Covalent Self-Assembly of Chloride- and Ion-Pair-Templated Cryptates.

Hollstein Selina S Shyshov Oleksandr O Hanževački Marko M Zhao Jie J Rudolf Tamara T Jäger Christof M CM von Delius Max M

Angewandte Chemie (International ed. in English) 20220512 28

While supramolecular hosts capable of binding and transporting anions and ion pairs are now widely available, self-assembled architectures are still rare, even though they offer an inherent mechanism for the release of the guest ion(s). In this work, we report the dynamic covalent self-assembly of tripodal, urea-based anion cryptates that are held together by two orthoester bridgeheads. These hosts exhibit affinity for anions such as Cl- , Br- or I- in the modera ...[more]

PMID: 35384202

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Project description:The future of materials chemistry will be defined by our ability to precisely arrange components that have considerably larger dimensions and more complex compositions than conventional molecular or macromolecular building blocks. However, exerting structural and constitutional control in the assembly of nanoscale entities presents a considerable challenge. Dynamic covalent nanoparticles are emerging as an attractive category of reaction-enabled solution-processable nanosized building block through which the rational principles of molecular synthetic chemistry can be extended into the nanoscale. From a mixture of two hydrazone-based dynamic covalent nanoparticles with complementary reactivity, specific molecular instructions trigger selective assembly of intimately mixed heteromaterial (Au-Pd) aggregates or materials highly enriched in either one of the two core materials. In much the same way as complementary reactivity is exploited in synthetic molecular chemistry, chemospecific nanoparticle-bound reactions dictate building block connectivity; meanwhile, kinetic regioselectivity on the nanoscale regulates the detailed composition of the materials produced. Selectivity, and hence aggregate composition, is sensitive to several system parameters. By characterizing the nanoparticle-bound reactions in isolation, kinetic models of the multiscale assembly network can be constructed. Despite ignoring heterogeneous physical processes such as aggregation and precipitation, these simple kinetic models successfully link the underlying molecular events with the nanoscale assembly outcome, guiding rational optimization to maximize selectivity for each of the three assembly pathways. With such predictive construction strategies, we can anticipate that reaction-enabled nanoparticles can become fully incorporated in the lexicon of synthetic chemistry, ultimately establishing a synthetic science that manipulates molecular and nanoscale components with equal proficiency.

Dataset Information

Dynamic Covalent Self-Assembly of Chloride- and Ion-Pair-Templated Cryptates.

Publications

Dynamic Covalent Self-Assembly of Chloride- and Ion-Pair-Templated Cryptates.

Similar Datasets

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