Metal-Peptide Torus Knots from Flexible Short Peptides

Inomata, Yuuki; Sawada, Tomohisa; Fujita, Makoto

doi:10.1016/j.chempr.2019.12.009

Cited by 118 publications

(85 citation statements)

References 35 publications

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“…Weavings, knots, links and related geometrical structures are currently of considerable interest in materials chemistry and biochemistry, as testified in recent reviews (Lim & Jackson, 2015;Flapan, 2015;Bruns & Stoddart, 2016;Pieters et al, 2016;Horner et al, 2016;Fielden et al, 2017) and in other recent reports (Danon et al, 2017;Wu et al, 2017;Kim et al, 2018;Zhang et al, 2018;Leigh et al, 2019;Sawada, Saito et al, 2019;Sawada, Inomata et al, 2019;Inomata et al, 2020). Suggested knots most suitable for self-assembly have recently been identified (Marenda et al, 2018).…”

Section: Knots and Linksmentioning

confidence: 99%

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Isogonal weavings on the sphere: knots, links, polycatenanes

O’Keeffe¹,

Treacy²

2020

Acta Cryst Sect A

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Mathematical knots and links are described as piecewise linear – straight, non-intersecting sticks meeting at corners. Isogonal structures have all corners related by symmetry (`vertex'-transitive). Corner- and stick-transitive structures are termed regular. No regular knots are found. Regular links are cubic or icosahedral and a complete account of these (36 in number) is given, including optimal (thickest-stick) embeddings. Stick 2-transitive isogonal structures are again cubic and icosahedral and also encompass the infinite family of torus knots and links. The major types of these structures are identified and reported with optimal embeddings. The relevance of this work to materials chemistry and biochemistry is noted.

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Section: Knots and Linksmentioning

confidence: 99%

“…They also feature prominently in the knots most amenable to construction by molecular self-assembly (Marenda et al, 2018). Notable recently achieved molecular examples are (4,3) (Danon et al, 2017), (8,3) (Kim et al, 2018), and (7,2) and (8,2) (Inomata et al, 2020).…”

Section: Knots and Links With Axial Symmetrymentioning

confidence: 99%

Isogonal weavings on the sphere: knots, links, polycatenanes

O’Keeffe¹,

Treacy²

2020

Acta Cryst Sect A

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“…NMR spectra were recorded on a Bruker Avance 200, a Bruker AvanceNeo 500, or a Bruker Avance 600 spectrometer, the latter being equipped with a cryogenically cooled triple-resonance probe head. Chemical shifts for 1 H, 13 C, and 19 F spectra are expressed in parts per million (ppm) and coupling constants (J) are reported in Hertz (Hz). 1 H and 13 C spectra of the diamagnetic compounds were referenced to TMS at 0.0 ppm and the chemical shifts of the paramagnetic complexes/cage are reported relative to the resonance of the residual methyl proton and carbon of CD3CN (δH = 1.94 ppm, δC = 1.32 ppm).…”

Section: Nmr Spectroscopymentioning

confidence: 99%

“…1 H and 13 C spectra of the diamagnetic compounds were referenced to TMS at 0.0 ppm and the chemical shifts of the paramagnetic complexes/cage are reported relative to the resonance of the residual methyl proton and carbon of CD3CN (δH = 1.94 ppm, δC = 1.32 ppm). 19 F spectra were referenced to C6F6 at -164.9 ppm. All measurements were carried out at 298 K unless reported otherwise.…”

Section: Nmr Spectroscopymentioning

confidence: 99%

A Paramagnetic NMR Spectroscopy Toolbox for the Characterisation of Paramagnetic/Spin-Crossover Coordination Complexes and Metal-Organic Cages

Lehr¹,

Paschelke²,

Trumpf³

et al. 2020

Preprint

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<div> The large paramagnetic shifts and short relaxation times resulting from the presence of a paramagnetic centre complicate NMR data acquisition and interpretation in solution. In contrast to the large number of standard NMR methods for diamagnetic compounds, the number of paramagnetic NMR methods is limited and spectral assignment often relies on theoretical models. We report a toolbox of 1D (1H, proton-coupled 13C, selective 1H‑decoupling 13C, steady-state NOE) and 2D (COSY, NOESY, HMQC) paramagnetic NMR methods for the straightforward structural characterisation of paramagnetic complexes in solution and demonstrate its general applicability for fields from coordination chemistry to spin‑crossover complexes and supramolecular chemistry through the characterisation of CoII and high-spin FeII mononuclear complexes as well as a Co4L6 cage. The toolbox takes advantage of the reduced signal overlap, decreased instrument time and greater sensitivity from the presence of the paramagnetic centre while overcoming the loss of structural information from the wide chemical shift dispersion and broad signals. In some circumstances, more structural information was revealed in the COSY spectra than would be observable for a diamagnetic analogue; as well as the expected through-bond cross-peaks, through-space and exchange cross-peaks were also observed for mononuclear complexes with multiple ligand environments and fast ligand exchange. With this toolbox, the standard characterisation of paramagnetic complexes and cages is now possible using NMR spectroscopic methods. </div>

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“…7 Knotting at the molecular level thus has major effects upon material properties. 8,9 Since Sauvage's first full characterisation of synthetic knotted molecules three decades ago, 10 the beauty of these woven architectures has attracted chemists, 11 leading to recent breakthroughs in the synthesis of complex, highly symmetric, knots, 12,13,14,15,16,17,18 and to investigations of their functions. 19,20 To date, synthetic routes to molecular knots and links have focussed on the preparation of highly symmetric knots with few crossing points, such as the threecrossing trefoil knot.…”

mentioning

confidence: 99%

Controlling the Shape and Chirality of an Eight-crossing Molecular Knot

Carpenter¹,

McTernan²,

Greenfield³

et al. 2020

Preprint

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The knotting of biomolecules impacts their function, and enables them to carry out new tasks. Likewise, complex topologies underpin the operation of many synthetic molecular machines. The ability to generate and control more complex knotted architectures is essential to endow these machines with more advanced functions. Here we report the synthesis of a molecular knot with eight crossing points, consisting of a single organic loop woven about six templating metal centres, via one-pot self-assembly from a simple pair of dialdehyde and diamine subcomponents and a single metal salt. The structure and topology of the knot were established by NMR spectroscopy, mass spectrometry and X-ray crystallography. Upon demetallation, the purely organic strand relaxes into a symmetric conformation, whilst retaining the topology of the original knot. This knot is topologically chiral, and may be synthesised diastereoselectively through the use of an enantiopure diamine building block.

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Metal-Peptide Torus Knots from Flexible Short Peptides

Cited by 118 publications

References 35 publications

Isogonal weavings on the sphere: knots, links, polycatenanes

Isogonal weavings on the sphere: knots, links, polycatenanes

A Paramagnetic NMR Spectroscopy Toolbox for the Characterisation of Paramagnetic/Spin-Crossover Coordination Complexes and Metal-Organic Cages

Controlling the Shape and Chirality of an Eight-crossing Molecular Knot

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