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

Research output: Contribution to journalArticle

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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