Fine‐Tuning of the Sequential Self‐Assembly of Entangled Polyhedra by Exploiting the Side‐Chain Effect DOI Open Access
Yuya Domoto,

Ren Nakabayashi,

Tatsuya Tsurumi

и другие.

Chemistry - An Asian Journal, Год журнала: 2024, Номер unknown

Опубликована: Дек. 30, 2024

Abstract The control of the sequential self‐assembly processes highly entangled (Ag 3 L 2 ) n ( =2,4,6,8) and Ag 21 12 coordination polyhedra using side‐chain effects was studied via introduction linear or branched side chains into tripodal ligands. In addition to changes in intermediate polyhedral species affording multi‐ pathway process, disruption kinetic observed, thus demonstrating utility steric for construction 3D‐entangled molecular materials on 5 nm scale with high complexity.

Язык: Английский

Non-statistical assembly of multicomponent [Pd2ABCD] cages DOI

Kai Wu,

Élie Benchimol, Ananya Baksi

и другие.

Nature Chemistry, Год журнала: 2024, Номер 16(4), С. 584 - 591

Опубликована: Янв. 19, 2024

Язык: Английский

Процитировано

63

Heteromeric Completive Self-Sorting in Coordination Cage Systems DOI
Élie Benchimol, Irene Regeni,

Bo Zhang

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(10), С. 6905 - 6911

Опубликована: Фев. 29, 2024

Heteroleptic coordination cages, nonstatistically assembled from a set of matching ligands, can be obtained by mixing individual components or via cage-to-cage transformations homoleptic precursors. Based on the latter approach, we here describe new level self-sorting in cage systems, namely, 'heteromeric completive self-sorting'. Here, two heteroleptic assemblies type Pd2A2B2 and Pd2A2C2, sharing one common ligand component A but differing other, are shown to coexist solution. This reached either statistical mixture based some ligands B C or, alternatively, following first step integrative giving distinct Pd2B2C2 intermediate. While subtle enthalpic factors dictate outcome self-sorting, found that it is controllable. From unique three demonstrate transition strict forming Pd2AB2C heteromeric give Pd2A2C2 variation ratio. Cage-to-cage were followed NMR MS experiments. Single crystal X-ray structures for cages obtained, impressively highlighting versatility form π-stacked trans-figure-of-eight arrangement occupy cis-edges only single edge Pd2AB2C. study paves way toward control populations systems chemistry context with emerging features such as chemical information processing, adaptive guest selectivity, stimuli-responsive catalytic action.

Язык: Английский

Процитировано

20

Supramolecular and molecular capsules, cages and containers DOI Creative Commons

C. Cox,

Jessica Hale,

Paulina Molinska

и другие.

Chemical Society Reviews, Год журнала: 2024, Номер 53(21), С. 10380 - 10408

Опубликована: Янв. 1, 2024

Stemming from early seminal notions of molecular recognition and encapsulation, three-dimensional, cavity-containing capsular compounds assemblies have attracted intense interest due to the ability modulate chemical physical properties species encapsulated within these confined spaces compared bulk environments. With such a diverse range covalent motifs non-covalent (supramolecular) interactions available assemble building blocks, an incredibly wide-range capsular-type architectures been developed. Furthermore, synthetic tunability internal environments gives chemists opportunity engineer systems for uses in sensing, sequestration, catalysis transport molecules, just name few. In this tutorial review, overview is provided into design principles, synthesis, characterisation, structural facets coordination cages, porous organic supramolecular capsules, foldamers mechanically interlocked molecules. Using recent examples, advantages limitations each system are explored, highlighting their application various tasks functions.

Язык: Английский

Процитировано

14

Diastereoselective Self‐Assembly of Low‐Symmetry PdnL2n Nanocages through Coordination‐Sphere Engineering** DOI Creative Commons
Paulina Molinska, Andrew Tarzia, Louise Male

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(51)

Опубликована: Окт. 27, 2023

Metal-organic cages (MOCs) are popular host architectures assembled from ligands and metal ions/nodes. Assembling structurally complex, low-symmetry MOCs with anisotropic cavities can be limited by the formation of statistical isomer libraries. We set out to investigate use primary coordination-sphere engineering (CSE) bias selectivity within homo- heteroleptic Pd

Язык: Английский

Процитировано

21

Highly Anisotropic Pd2Lab2Lcc2 and Pd2Lab2Lcd2 Type Cages by Heteromeric Completive Self‐Sorting DOI

Minaz Parbin,

Vellaiyadevan Sivalingam, Dillip Kumar Chand

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Авг. 20, 2024

Pd(II)-based low-symmetry coordination cages possessing anisotropic cavities are of great interest. The common strategies employed to achieve such utilize either more than one type symmetrical ligands (e.g., L

Язык: Английский

Процитировано

9

Shape‐Complementary Multicomponent Assembly of Low‐Symmetry Co(III)Salphen‐Based Coordination Cages DOI Creative Commons
Bo Zhang, Haeri Lee, Julian J. Holstein

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(24)

Опубликована: Апрель 4, 2024

Abstract While metal‐mediated self‐assembly is a popular technique to construct discrete nanosized objects, highly symmetric structures, built from one type of ligand at time, are dominating reported systems. The tailored integration set different ligands requires sophisticated approaches avoid narcissistic separation or formation statistical mixtures. Here, we demonstrate how the combination three structure‐guiding effects (metal‐templated macrocyclization, additional bridging and shape‐complementarity) based on Co(III)salphen metal nodes allows for rational high‐yielding synthesis structurally complex, lantern‐shaped cages with up four differentiable bridges. Three new heteroleptic coordination dinuclear macrocycles were synthesized in one‐pot reaction approach fully characterized, including single crystal X‐ray analyses. One cage groups two same ligands, another around Co 2 ‐bis‐salphen ring. In most complex structure, this ring unsymmetric, rendering all connections between centers distinguishable. assembly Pd(II) has been shown be dynamic, beneficial cage‐to‐cage transformations, cascades adaptive systems, herein introduced kinetically more inert will advantageous applications enzyme‐like catalysis molecular machinery that require enhanced structural chemical stability.

Язык: Английский

Процитировано

8

Triply Adaptive Libraries of Dynamic Covalent Macrocycles: Switching between Sorted and Unsorted States DOI
Zhaozheng Yang, Ferran Esteve, Cyril Antheaume

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(22), С. 15438 - 15445

Опубликована: Май 27, 2024

Dynamic noncovalent and covalent chemistries have enabled the constitutional modulation of chemical entities within dynamic systems. The switching between order disorder, i.e., self-sorted unsorted states libraries, remains challenging. Herein, we study adaptive behaviors a library imine macrocycles generated from dialdehydes diamines, seeking ways to exert control over sorting unsorting processes. distribution constituents in present is modulated response internal external effectors (e.g., time, metal cations, fuels), resulting transient amplification out-of-equilibrium states. showcases higher complexity systems subject multiple adaptation through interconversion singularity/order diversity/disorder.

Язык: Английский

Процитировано

8

Host–guest complexation‐induced chirality switching of pillararenes by perylene diimide‐based hexagonal metallacages DOI Creative Commons

Yali Hou,

Chaoqun Mu,

Yunzhi Shi

и другие.

Aggregate, Год журнала: 2024, Номер unknown

Опубликована: Июнь 27, 2024

Abstract Chirality in confined nanospaces has brought some new insights into chirality transfer, amplification, and chiroptical properties. However, switching, which is a common phenomenon biological systems, never been realized environments. Herein, we report type of hexagonal metallacages that shows good host–guest interactions with ethoxy pillar[5]arene pillar[6]arene, as confirmed by single‐crystal X‐ray analysis. Importantly, when chiral pillar[5]arene‐based molecular universal joint (MUJ) used the guest, complexation would drive alkyl ring MUJ flip from outside to inside cavity its unit, enables configuration change along inversion MUJ. Moreover, facilitates transfer guests hosts, giving circularly polarized luminescence system. This study provides unique metallacage‐pillararene recognition motif for switching planar pillararenes, will promote construction systems tunable advanced applications.

Язык: Английский

Процитировано

6

Host–Guest Interactions Induced Enhancement in Oxidase-Like Activity of a Benzothiadiazole Dye Inside an Aqueous Pd8L4 Barrel DOI
Debsena Chakraborty, Navjot Kaur,

Jagabandhu Sahoo

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(36), С. 24901 - 24910

Опубликована: Авг. 28, 2024

The effect of host–guest interactions on the chemistry encapsulated molecules is a fascinating field research that has gained momentum in recent years. Much work this been focused such catalysis and photoluminescence dyes. However, related photoinduced processes, as photoregulated oxidase-mimicking activity, not explored much. Herein, we report unique example enhancement oxidase-like activity benzothiadiazole dye (G1) water through encapsulation within M8L4 molecular barrel (1). Favorable helped guest G1 to have better electron transfer oxygen leading increased production superoxide radical anions activity. Furthermore, inside 1 also caused change redox potentials which after produced oxidizing agent than free G1. These phenomena combined enhance upon cage 1. present demonstrates processes.

Язык: Английский

Процитировано

6

The beauty of low symmetry: Non-statistical assembly of [Pd2(LA)(LB)(LC)(LD)]4+ cages DOI Creative Commons
L Faulkner, James D. Crowley

Chem, Год журнала: 2024, Номер 10(2), С. 440 - 442

Опубликована: Янв. 31, 2024

Язык: Английский

Процитировано

5