Efficient Hydrogen Photoproduction in Water with Hybrid Systems Composed of Quantum Dots and Molecular Catalysts
Martina Sandroni a b, Jérôme Fortage b, Marie-Noëlle Collomb b, Peter Reiss a, Dmitry Aldakov a
a UMR5819 SyMMES CEA-CNRS-UGA CEA-Grenoble INAC/SyMMES, Avenue des Martyrs, 17, Grenoble, France
b DCM, Univ. Grenoble Alpes, CNRS, France, Grenoble, France
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2018 (NFM18)
S1 Solar Fuel 18
Torremolinos, Spain, 2018 October 22nd - 26th
Organizers: Shannon Boettcher and Kevin Sivula
Oral, Dmitry Aldakov, presentation 240
DOI: https://doi.org/10.29363/nanoge.nfm.2018.240
Publication date: 6th July 2018

Semiconductor nanocrystals (quantum dots) emerged in the last years as an appealing alternative to molecular photosensitizers, owing to their superior stability, intense light absorption and bright luminescence. In particular, non-cadmium quantum dots seem to be a particularly interesting choice as they display good optoelectronic properties while containing no toxic elements with respect to CdSe and CdTe.[1] In the field of artificial photosynthesis, very efficient ”hybrid” photocatalytic systems for hydrogen production in water were obtained by associating Cd-based quantum dots as photosensitizers with molecular H2-evolving catalysts in presence of a sacrificial reductant. [2,3]

In this communication, we describe new hybrid systems associating environmentally friendly (Cd-free) quantum dots with molecular catalysts based on earth-abundant metals, in order to perform photocatalytic H2 production in purely aqueous environment.

Core-shell CuInS2/ZnS nanocrystals capped with glutathione were synthesized in the aqueous phase, and their structural and optical properties were fully characterized. The nanocrystals exhibit a broad absorption throughout the visible range with orange luminescence in aqueous solution. For the photocatalysis process the colloidal solution was mixed with a cobalt macrocyclic catalyst and a sacrificial reductant, and the H2 production under irradiation was quantified by gas chromatography. This hybrid system exhibited remarkable activity for hydrogen production under visible light irradiation at pH 5.0 with up to 7700 and 1010 turnover numbers versus catalyst and QDs, respectively. The CIS/ZnS nanoparticles were also compared to widely studied CdSe nanocrystals, using the same catalyst, and the former give remarkably better performances in terms of TON. [4]

 

1. M. Sandroni et al. ACS Energy Lett., 2017, 2, 1076–1088.

2. C. Gimbert-Suriñach et al., J. Am. Chem. Soc. 2014, 136, 7655-7661.

3. Z.J. Han et al., Science 2012, 338, 1321-1324

4. M. Sandroni et al. Energy Environ. Sci., 2018, DOI: 10.1039/c8ee00120k.

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