Direct Construction of Magnetic and Electrical Two-Dimensional Radical Covalent Organic Frameworks.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 42337248.
- Also identified by DOI 10.1038/s41467-026-74618-4 and PMC identifier 13291238.
- Licence recorded as CC BY-NC-ND.
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Abstract
Radicals arranged in a two-dimensional (2D) hexagonal network can offer various exotic magnetic, electronic, and optical properties that find application in electronics/spintronics. However, direct synthesis remains challenging due to the scarcity of stable, symmetry-matched radical building blocks. Here, we report the bottom-up synthesis of hexagonal 2D radical covalent organic frameworks (RCOFs) with unpaired electrons at the nodes of the frameworks. A planar verdazyl radical amine (V-NH<sub>2</sub>) undergoes Schiff-base condensation with aldehydes to afford highly crystalline hexagonal RCOFs (VTPT and VPMT). The spin density was precisely controlled through the selection of building blocks with modulated spin-spin distances. The EPR and SQUID measurements confirmed a high spin concentration with antiferromagnetic interactions at low temperature, which is further tuned by interlayer interactions. Thin films of VTPT exhibited preferential in-plane orientation with enhanced photoconductivity, attributed to improved π-conjugation. These findings establish a direct route to RCOFs and underscore their potential as pseudo 1-dimensional antiferromagnetic materials.