Hierarchical organization of perylene bisimides and polyoxometalates for photo-assisted water oxidation

Marcella Bonchio*, Zois Syrgiannis, Max Burian, Nadia Marino, Erica Pizzolato, Konstantin Dirian, Francesco Rigodanza, Giulia Alice Volpato, Giuseppina La Ganga, Nicola Demitri, Serena Berardi, Heinz Amenitsch, Dirk M Guldi, Stefano Caramori, Carlo Alberto Bignozzi, Andrea Sartorel, Maurizio Prato*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

The oxygen in Earth's atmosphere is there primarily because of water oxidation performed by photosynthetic organisms using solar light and one specialized protein complex, photosystem II (PSII). High-resolution imaging of the PSII 'core' complex shows the ideal co-localization of multi-chromophore light-harvesting antennas with the functional reaction centre. Man-made systems are still far from replicating the complexity of PSII, as the majority of PSII mimetics have been limited to photocatalytic dyads based on a 1:1 ratio of a light absorber, generally a Ru-polypyridine complex, with a water oxidation catalyst. Here we report the self-assembly of multi-perylene-bisimide chromophores (PBI) shaped to function by interaction with a polyoxometalate water-oxidation catalyst (Ru4POM). The resulting [PBI]5Ru4POM complex shows a robust amphiphilic structure and dynamic aggregation into large two-dimensional paracrystalline domains, a redshifted light-harvesting efficiency of >40% and favourable exciton accumulation, with a peak quantum efficiency using 'green' photons (λ > 500 nm). The modularity of the building blocks and the simplicity of the non-covalent chemistry offer opportunities for innovation in artificial photosynthesis.

Original languageEnglish
Pages (from-to)146-153
Number of pages8
JournalNature Chemistry
Volume11
Issue number2
DOIs
Publication statusPublished - 2019

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Chemistry(all)

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