Chemical engineering of quasicrystal approximants in lanthanide-based coordination solids

Voigt, Laura; Kubus, Mariusz; Pedersen, Kasper S.

doi:10.1038/s41467-020-18328-5

Cited by 15 publications

(19 citation statements)

References 60 publications

(74 reference statements)

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“…9 We recently reported the utilization of trans-{Yb II I 2 } nodes as five-vertex building units to form the triangular elongated tiling in Yb II I 2 (bipy) 5/2 (bipy = 4,4′-bipyridine). 10 The lanthanide ions are particularly relevant for the realization of both ATs and ddQC phases as the coordinative plasticity allows for their incorporation in a variety of local coordination geometries. Furthermore, their weak interactions with ligands are commensurate with the weak interactions typically intrinsic to aperiodic structures.…”

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confidence: 99%

Magnetic Archimedean Tessellations in Metal–Organic Frameworks

et al. 2021

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The self-assembly of lanthanide ions with ditopic organic spacers results in the formation of complex tiling patterns that mimic the structural motifs of quasi-periodic 2D materials. The linking of trans-{LnI 2 } + nodes (Ln = Gd, Dy) by both closedshell and anion radicals of 4,4′-bipyridine affords rare examples of Archimedean tessellations in a metal−organic framework. We furthermore demonstrate the occurrence of sizable magnetic exchange interactions and slow relaxation of magnetization behavior in a complex tessellation pattern. The implementation of Archimedean tessellations in lanthanide(III) coordination solids couriers a strategy to design elusive quasi-periodic metal−organic frameworks with inimitable magnetic properties.T he design of complex and aperiodic two-dimensional tessellations in molecule-based materials constitutes a novel route to harvest physical properties, for instance, photonic, electronic, magnetic, and phononic characteristics, which are expected to be unparalleled compared to their periodic counterparts. 1−3 However, applications are elusive due to the severe scarcity of materials exhibiting the desired structural motifs. The two-dimensional dodecagonal quasicrystalline phase (Figure 1a, ddQC) is well-known in both hard and soft materials as well as in supramolecular networks. 4−6 In these system, the tessellation of triangles and squares, at a ratio of 4/√3 ≈ 2.3, leads to the disappearance of periodicity and the formation of local 12-fold rotational symmetry. Generally, quasicrystals are found in the vicinity of structurally related, periodic structures, and the ddQCs often co-occur with the periodic Archimedean tessellations (ATs, Figure 1b,c), which are termed quasicrystal approximants. 7 The sole example of a quasicrystal phase found in a metal−organic network structure

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Magnetic Archimedean Tessellations in Metal–Organic Frameworks

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“…Most of the them deals with molecular assembly -fullerenes organised as 2D small patches of a quasicrystalline triangle-square tiling on Pt 3 Ti(111) 23 and molecules aperiodically organised by Ce-directed assembly on Ag(111). 24,25 The case of the 2D Oxide QuasiCrystals (OQCs) on dense metallic surfaces remains unique. 13 The stoichiometric ratio and concentration, as well as the coordinative plasticity, charge and ionic radii of cations, are invoked as key parameters towards the formation of quasiperiodic films.…”

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confidence: 99%

Two-dimensional oxide quasicrystal approximants with tunable electronic and magnetic properties

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“…The batch‐to‐batch variation, along with its low in planta abundance, [1, 7] spurred its total synthesis which was a success in chemistry despite the inevitable harsh condition and poor yield [10] . Furthermore, the knowledge about factors that stymie the Hyp expression in Hypericum plants remains largely unknown, [3] thereby bottlenecking its scalable production by current approaches such as synthetic biology strategy [11] . These observations necessitate biosustainable and innovative solutions to the Hyp regeneration issue.…”

Section: Introductionmentioning

confidence: 99%

Regeneration of Phytochemicals by Structure‐Driven Organization of Microbial Biosynthetic Steps

Guan

Han

et al. 2021

Angewandte Chemie

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Medicinal phytochemicals, such as artemisinin and taxol, have impacted the world, and hypericin might do so if its availability issue could be addressed. Hypericin is the hallmark component of Saint John's wort (Hypericum perforatum L.), an approved depression alleviator documented in the US, European, and British pharmacopoeias with its additional effectiveness against diverse cancers and viruses. However, the academia‐to‐industry transition of hypericin remain hampered by its low in planta abundance, unfeasible bulk chemical synthesis, and unclear biosynthetic mechanism. Here, we present a strategy consisting of the hypericin‐structure‐centered modification and reorganization of microbial biosynthetic steps in the repurposed cells that have been tamed to enable the designed consecutive reactions to afford hypericin (43.1 mg L−1), without acquiring its biosynthetic knowledge in native plants. The study provides a synthetic biology route to hypericin and establishes a platform for biosustainable access to medicinal phytochemicals.

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Chemical engineering of quasicrystal approximants in lanthanide-based coordination solids

Cited by 15 publications

References 60 publications

Magnetic Archimedean Tessellations in Metal–Organic Frameworks

Magnetic Archimedean Tessellations in Metal–Organic Frameworks

Two-dimensional oxide quasicrystal approximants with tunable electronic and magnetic properties

Regeneration of Phytochemicals by Structure‐Driven Organization of Microbial Biosynthetic Steps

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