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Design and synthesis of two-dimensional covalent organic frameworks with four-arm cores: prediction of remarkable ambipolar charge-transport properties

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Abstract

We have considered three two-dimensional (2D) π-conjugated polymer network (i.e., covalent organic frameworks, COFs) materials based on pyrene, porphyrin, and zinc-porphyrin cores connected via diacetylenic linkers. Their electronic structures, investigated at the density functional theory global-hybrid level, are indicative of valence and conduction bands that have large widths, ranging between 1 and 2 eV. Using a molecular approach to derive the electronic couplings between adjacent core units and the electron-vibration couplings, the three π-conjugated 2D COFs are predicted to have ambipolar charge-transport characteristics with electron and hole mobilities in the range of 65–95 cm2 V−1 s−1. Such predicted values rank these 2D COFs among the highest-mobility organic semiconductors. In addition, we have synthesized the zinc-porphyrin based 2D COF and carried out structural characterization via powder X-ray diffraction, high-resolution transmission electron microscopy, and surface area analysis, which demonstrates the feasibility of these electroactive networks. Steady-state and flash-photolysis time-resolved microwave conductivity measurements on the zinc-porphyrin COF point to appreciable, broadband photoconductivity while transmission spectral measurements are indicative of extended π-conjugation.

Graphical abstract: Design and synthesis of two-dimensional covalent organic frameworks with four-arm cores: prediction of remarkable ambipolar charge-transport properties

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Publication details

The article was received on 08 Jan 2019, accepted on 22 May 2019 and first published on 22 May 2019


Article type: Communication
DOI: 10.1039/C9MH00035F
Mater. Horiz., 2019, Advance Article

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    Design and synthesis of two-dimensional covalent organic frameworks with four-arm cores: prediction of remarkable ambipolar charge-transport properties

    S. Thomas, H. Li, R. R. Dasari, A. M. Evans, I. Castano, T. G. Allen, O. G. Reid, G. Rumbles, W. R. Dichtel, N. C. Gianneschi, S. R. Marder, V. Coropceanu and J. Brédas, Mater. Horiz., 2019, Advance Article , DOI: 10.1039/C9MH00035F

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