We report the synthesis of crystalline two-dimensional covalent organic frameworks (COFs) by connecting hydroxybenzene-aldehyde and acetonitrile building blocks to form cyano-substituted benzofuran linkages. Unlike the majority of COFs that were synthesized based on condensation reactions, the COFs in this report are crystallized from irreversible cascade reactions involving consecutive cyanide migration, ring-closure, and oxidation reactions. The irreversible property endows the COFs with high chemical stability in both acid and base and allows them to be postsynthetically modified to install predesigned functionality under harsh conditions. We highlight that the functionalized COFs serve as exceptional vehicles for superprotonic conductions.

A cyano-substituted styrene derivative is synthesized and successfully prepared to lamellate single crystals through precisely controlling the crystal growth conditions. The lamellate single crystals with regular edge and smooth surface display intrinsically ordered stacking and high quality, all of which are of importance for high optoelectronic performance. The single-component light-emitting transistors based on the lamellate crystals offer striking device performance in terms of record external quantum efficiency of 2.02%, exceeding the benchmark value in this field. Such organic lightemitting single crystals provide a versatile platform for designing and engineering their structures and optoelectronic properties toward light-emitting devices.

A novel organic conjugated molecule was synthesised and fabricated into sheet-shaped crystals. The micro/nano-sheets show an excellent hydrogen evolution rate (8143 μmol g−1 h−1) from water splitting, outperforming most organic photocatalysts.

We report the preparation of two high-quality lamellar crystals of cayno-substituted p-phenylene vinylene derivatives and the fabrication of their transistors. The transistors were demonstrated hysteresis-free, low subthreshold swing of 0.10...