Ruthenium based photosensitizer/catalyst supramolecular architectures in light driven water oxidation

Max Burian, Zois Syrgiannis, Giuseppina La Ganga, Fausto Puntoniero, Mirco Natali, Sebastiano Campagna, Maurizo Prato, Marcella Bonchio, Heinz Amenitsch, Andrea Sartorel

Research output: Contribution to journalArticleResearchpeer-review

Abstract

Light driven water oxidation is a key step in artificial photosynthesis, aimed at splitting water into hydrogen and oxygen with sunlight. In such process, the interactions between a photosensitizer (PS) and a water oxidation catalyst (WOC) play a crucial role in the rates of photoinduced electron transfers, determining the overall quantum efficiency of the system. In this work, by means of Small Angle X-ray Scattering (SAXS) we investigate the nature of the aggregates between ruthenium polypyridine photosensitizers (Rubpy and Ru4dend) and a tetraruthenium polyoxometalate (Ru4POM) water oxidation catalyst. Aggregate scattering is confirmed by the strong intensity-increase in the low-q regime, whereas the power law-fit of this region show slopes between −3 and −4, suggesting globular and porous aggregates. Intermolecular PS/WOC distances lower than 3 nm support the observed fast photoinduced electron transfers (<120 ps), however the proximity of the two components in the hybrids is also responsible for fast charge recombination. Approaches for inhibiting such undesired process are discussed.
Original languageEnglish
Pages (from-to)171-175
JournalInorganica chimica acta
DOIs
Publication statusPublished - 1 Jan 2017

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Photosensitizing Agents
Photosensitizers
Ruthenium
ruthenium
catalysts
Oxidation
oxidation
Catalysts
Water
water
electron transfer
water splitting
photosynthesis
sunlight
scattering
Photosynthesis
Electrons
proximity
quantum efficiency
X ray scattering

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Fields of Expertise

  • Advanced Materials Science

Cite this

Ruthenium based photosensitizer/catalyst supramolecular architectures in light driven water oxidation. / Burian, Max; Syrgiannis, Zois; La Ganga, Giuseppina; Puntoniero, Fausto; Natali, Mirco; Campagna, Sebastiano; Prato, Maurizo; Bonchio, Marcella; Amenitsch, Heinz; Sartorel, Andrea.

In: Inorganica chimica acta, 01.01.2017, p. 171-175.

Research output: Contribution to journalArticleResearchpeer-review

Burian, M, Syrgiannis, Z, La Ganga, G, Puntoniero, F, Natali, M, Campagna, S, Prato, M, Bonchio, M, Amenitsch, H & Sartorel, A 2017, 'Ruthenium based photosensitizer/catalyst supramolecular architectures in light driven water oxidation' Inorganica chimica acta, pp. 171-175. https://doi.org/10.1016/j.ica.2016.04.010
Burian, Max ; Syrgiannis, Zois ; La Ganga, Giuseppina ; Puntoniero, Fausto ; Natali, Mirco ; Campagna, Sebastiano ; Prato, Maurizo ; Bonchio, Marcella ; Amenitsch, Heinz ; Sartorel, Andrea. / Ruthenium based photosensitizer/catalyst supramolecular architectures in light driven water oxidation. In: Inorganica chimica acta. 2017 ; pp. 171-175.
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AU - Natali, Mirco

AU - Campagna, Sebastiano

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AB - Light driven water oxidation is a key step in artificial photosynthesis, aimed at splitting water into hydrogen and oxygen with sunlight. In such process, the interactions between a photosensitizer (PS) and a water oxidation catalyst (WOC) play a crucial role in the rates of photoinduced electron transfers, determining the overall quantum efficiency of the system. In this work, by means of Small Angle X-ray Scattering (SAXS) we investigate the nature of the aggregates between ruthenium polypyridine photosensitizers (Rubpy and Ru4dend) and a tetraruthenium polyoxometalate (Ru4POM) water oxidation catalyst. Aggregate scattering is confirmed by the strong intensity-increase in the low-q regime, whereas the power law-fit of this region show slopes between −3 and −4, suggesting globular and porous aggregates. Intermolecular PS/WOC distances lower than 3 nm support the observed fast photoinduced electron transfers (<120 ps), however the proximity of the two components in the hybrids is also responsible for fast charge recombination. Approaches for inhibiting such undesired process are discussed.

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