Influence of axle length on the rate and mechanism of shuttling in rigid H-shaped [2]rotaxanes

Gholami, Ghazale; Zhu, Kelong; Baggi, Giorgio; Schott, Eduardo; Zárate, Ximena

doi:10.1039/c7sc03736h

Cited by 38 publications

(37 citation statements)

References 26 publications

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“…Hirose and co‐workers investigated shuttling of crown ether rings in a series of [2]rotaxanes consisting of axles with two equivalent cationic ammonium stations connected by linear rigid rod‐like oligo‐paraphenylene linkers and found that the shuttling rate did not depend on the length of the spacer . Loeb and co‐workers also investigated shuttling of crown ether rings by varying the number of phenyl rings in the spacer—both charged and neutral systems . However, to the best of our knowledge, clear spacer effects have not been reported in [2]rotaxane systems with simple flexible alkyl and oligo(ethylene oxide) chain spacers connecting the two stations.…”

Section: Figurementioning

confidence: 99%

Spacer Length‐Independent Shuttling of the Pillar[5]arene Ring in Neutral [2]Rotaxanes

Ogoshi

Kotera

Nishida

et al. 2018

Chemistry A European J

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For a series of neutral [2]rotaxanes consisting of a pillar[5]arene ring and axles possessing two stations separated by flexible spacers of different lengths, the free energies of activation for the ring shuttling between the stations were found to be independent of the spacer length. The constitution of the spacer affects the activation energies: replacement of CH2 groups by repulsive oxygen atoms in the axle increases the barrier. The explanation for the observed length‐independence lies in the presence of a barrier for re‐forming the stable co‐conformation, which makes the ring travel back and forth along the thread in an intermediate state.

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Section: Figurementioning

confidence: 99%

Spacer Length‐Independent Shuttling of the Pillar[5]arene Ring in Neutral [2]Rotaxanes

Ogoshi

Kotera

Nishida

et al. 2018

Chemistry A European J

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“…It should be noted that a lengthy [2]rotaxane has been mounted inside the large cavities of NU-1000 via SALI and functions as a redox active molecular switch. 31 An alternative strategy is to use a design that positions the track of the molecular shuttle between the linker struts-i.e., on the crossbar of an H-shaped linker [33][34][35][36] (Figure 3C). This design was first used by Loeb, Schurko, and co-workers to make UWDM-4 and install a thermally driven, degenerate molecular shuttle inside a MOF with Zn 4 O nodes.…”

Section: The Bigger Picturementioning

confidence: 99%

Integrating the Mechanical Bond into Metal-Organic Frameworks

Wilson

Loeb

2020

Chem

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This perspective explores the idea of using mechanical bonds in the design and construction of metal-organic framework (MOF) materials.We provide examples of how and why mechanical bonds have been used in MOFs to date and examine different ways the mechanical bond can be incorporated into a MOF linker. Furthermore, we suggest ways that linkers with mechanical bonds could be used for the creation of MOFs with interesting topologies and properties dictated by the interlocked nature and dynamics of the mechanical bond.

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“…While there are a wealth of innovative molecular switches and machines based on mechanically interlocked molecules (e.g., rotaxanes, catenanes) that operate in solution [1][2][3][4][5][6], transferring their motion to the solid-state requires additional design features [7,8]. Components with both rigid and flexible structures are needed such that the mobile (flexible) units can be placed within or tethered to an ordered (rigid) skeletal structure.…”

Section: Introductionmentioning

confidence: 99%

Applying reticular synthesis to the design of Cu-based MOFs with mechanically interlocked linkers

et al. 2020

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The concept of "robust dynamics" describes the incorporation of mechanically interlocked molecules (MIMs) into metal-organic framework (MOF) materials such that large amplitude motions (e.g., rotation or translation of a macrocycle) can occur inside the free volume pore of the MOF. To aid in the preparation of such materials, reticular synthesis was used herein to design rigid molecular building blocks with predetermined ordered structures starting from the well-known MOF NOTT-101. New linkers were synthesized that have a T-shape, based on a triphenylene tetra-carboxylate strut, and their incorporation into Cu(II)-based MOFs was investigated. The single-crystal structures of three new MOFs, UWCM-12 (fof), β-UWCM-13 (loz), UWCM-14 (lil), with naked T-shaped linkers were determined; β-UWCM-13 is the first reported example of the loz topology. A fourth MOF, UWDM-14 (lil) is analogous to UWCM-14 (lil) but contains a [2]rotaxane linker. Variable-temperature, 2 H solid-state NMR was used to probe the dynamics of a 24-membered macrocycle threaded onto the MOF skeleton.

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Influence of axle length on the rate and mechanism of shuttling in rigid H-shaped [2]rotaxanes

Cited by 38 publications

References 26 publications

Spacer Length‐Independent Shuttling of the Pillar[5]arene Ring in Neutral [2]Rotaxanes

Spacer Length‐Independent Shuttling of the Pillar[5]arene Ring in Neutral [2]Rotaxanes

Integrating the Mechanical Bond into Metal-Organic Frameworks

Applying reticular synthesis to the design of Cu-based MOFs with mechanically interlocked linkers

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