Journal
NATURE CHEMISTRY
Volume 13, Issue 8, Pages 730-+Publisher
NATURE RESEARCH
DOI: 10.1038/s41557-021-00709-y
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Funding
- Nanosystems-Initiative-Munich Cluster of Excellence
- Deutsche Forschungsgemeinschaft [LA 1842/9-1]
- Swedish Research Council
- Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Linkoping University) [2009 00971]
- Knut and Alice Wallenberg Foundation
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The study focuses on the synthesis of ordered porous two-dimensional polymers on alkane-passivated graphite surfaces through two-staged photopolymerization. The highly ordered monolayer structures are first formed by self-assembly, followed by complete covalent cross-linking induced by violet light irradiation.
The use of solid supports and ultra-high vacuum conditions for the synthesis of two-dimensional polymers is attractive, as it can enable thorough characterization, often with submolecular resolution, and prevent contamination. However, most on-surface polymerizations are thermally activated, which often leads to high defect densities and relatively small domain sizes. Here, we have obtained a porous two-dimensional polymer that is ordered on the mesoscale by the two-staged topochemical photopolymerization of fluorinated anthracene triptycene (fantrip) monomers on alkane-passivated graphite surfaces under ultra-high vacuum. First, the fantrip monomers self-assemble into highly ordered monolayer structures, where all anthracene moieties adopt a suitable arrangement for photopolymerization. Irradiation with violet light then induces complete covalent cross-linking by [4+4] photocycloaddition to form a two-dimensional polymer, while fully preserving the long-range order of the self-assembled structure. The extent of the polymerization is confirmed by local infrared spectroscopy and scanning tunnelling microscopy characterization, in agreement with density functional theory calculations, which also gives mechanistic insights.
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