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Covalent organic frameworks are currently arousing considerable interest due to their desirable properties for a wide range of applications. Here, Jiang et al. report two such materials with triangular topologies which exhibit high hole mobility arising from extensive π-cloud delocalisation.

The design of covalent organic frameworks featuring high porosity and excellent charge transfer properties is crucial for widespread applications. Here, the authors report covalent organic frameworks with tunable dimensionality allowing to fine-tune their electronic band structure, charge mobility, and porosity.

The structures of amorphous MOFs are challenging to characterise. Here the authors use electron microscopy and pair distribution function methods, coupled with a polymerisation-based algorithm to determine the atomic structure of Fe-BTC, demonstrating the power of this computational approach.

Covalent organic frameworks can utilize π-stacking interactions for the formation of ordered, layered frameworks. Here, the authors report an ordered framework with tailored π-interactions resulting in periodic ordering in three dimensions, which leads to enhanced stability and electronic properties.

Covalent organic frameworks are crystalline porous polymers integrating molecular building blocks into periodic structures. Here, the authors report a general multiple-component condensation strategy that enables the use of one knot and two or three linkers to synthesize complex, anisotropic frameworks.

Controlling the number of molecular switches and their relative positioning within porous materials is critical to their functionality and properties. Here the authors systematically control the number of spiropyran units in a covalent organic framework using a mixed-linker synthetic strategy which resulted in one photoresponsive unit per pore.

It is difficult to prepare 2D polymers that are crystalline over large areas. Now, few-layer 2D polyimides and polyamides with good crystallinity on the micrometre scale have been synthesized on a water surface. A surfactant monolayer is used to organize amine monomers before their polymerization with anhydride moieties.

Development of porous proton-transporting materials combining stability and high performance has remained a challenge. Here, the authors report a stable covalent organic framework with excellent proton conductivity in which nitrogen sites on pore walls confine and stabilize a H3PO4 network in the channels via hydrogen-bonding interactions.