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Designed synthesis of stable light-emitting two-dimensional sp2 carbon-conjugated covalent organic frameworks.

ABSTRACT: Covalent organic frameworks enable the topological connection of organic chromophores into ? lattices, making them attractive for creating light-emitting polymers that are predesignable for both the primary- and high-order structures. However, owing to linkages, covalent organic frameworks are either unstable or poor luminescent, leaving the practical synthesis of stable light-emitting frameworks challenging. Here, we report the designed synthesis of sp2 carbon-conjugated frameworks that combine stability with light-emitting activity. The C=C linkages topologically connect pyrene knots and arylyenevinylene linkers into two-dimensional all sp2 carbon lattices that are designed to be ? conjugated along both the x and y directions and develop layer structures, creating exceptionally stable frameworks. The resulting frameworks are capable of tuning band gap and emission by the linkers, are highly luminescent under various conditions and can be exfoliated to produce brilliant nanosheets. These results suggest a platform based on sp2 carbon frameworks for designing robust photofunctional materials.

SUBMITTER: Jin E

PROVIDER: S-EPMC6175883 | biostudies-other | 2018 Oct

REPOSITORIES: biostudies-other

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Designed synthesis of stable light-emitting two-dimensional sp<sup>2</sup> carbon-conjugated covalent organic frameworks.

Jin Enquan E Li Juan J Geng Keyu K Jiang Qiuhong Q Xu Hong H Xu Qing Q Jiang Donglin D

Nature communications 20181008 1

Covalent organic frameworks enable the topological connection of organic chromophores into π lattices, making them attractive for creating light-emitting polymers that are predesignable for both the primary- and high-order structures. However, owing to linkages, covalent organic frameworks are either unstable or poor luminescent, leaving the practical synthesis of stable light-emitting frameworks challenging. Here, we report the designed synthesis of sp<sup>2</sup> carbon-conjugated frameworks t ...[more]

PMID: 30297692

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Project description:We use first-principles calculations to show that the square symmetry of two-dimensional (2D) metal-organic frameworks (MOFs) made from octaamino-substituted phthalocyanines and square planar Ni2+ ions, which enable strong conjugation of π electrons, has a critical impact on the magnetic properties of the lattice. In particular, we predict the unexpected emergence of a rare high-temperature ferromagnetic half-metallic ground state in one case. Among charge neutral MOFs made from (2,3,9,10,16,17,23,24)-octaiminophthalocyanine (OIPc) metallated with divalent first-row transition metal ions (M-OIPc; M = Cr2+, Mn2+, Fe2+, Co2+, Ni2+, Cu2+, Zn2+) and connected through square planar Ni-bisphenylenediimine moieties, NiMn-OIPc exhibits a half-metallic and ferromagnetic ground state with a large exchange energy resulting from the unique strong hybridization between the d/π orbitals of Mn, the Pc ring, and the Ni-bisphenylenediimine nodes. Notably, we show that for NiMn-OIPc there is a considerable difference between the ferromagnetic ordering temperature (Tc) predicted by a 2D Ising model, which exceeds 600 K, and a Tc of 170 K predicted by our more realistic Monte Carlo simulation that includes magnetic anisotropy. Critically, our simulations adopt two spin models that incorporate magnetic anisotropy in the form of exchange anisotropy and single-ion anisotropy. We further show that in the bulk, 2D layers of NiMn-OIPc adopt a slipped-parallel stacking configuration, and exhibit interlayer magnetic coupling that is sensitive to the relative in-plane displacement between adjacent layers. These results highlight the critical role of magnetic anisotropy in modeling the properties of 2D magnetic systems. More generally, it demonstrates that strong hybridization between open-shell ions and delocalized aromatic π systems with appropriate symmetry, combined with large magnetic anisotropy, will be an effective design strategy to realize ferromagnetic 2D MOFs with high Tc.

Dataset Information

Designed synthesis of stable light-emitting two-dimensional sp2 carbon-conjugated covalent organic frameworks.

Publications

Designed synthesis of stable light-emitting two-dimensional sp<sup>2</sup> carbon-conjugated covalent organic frameworks.

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