Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.072
Publication date: 18th July 2019
Artificial photosynthesis represents a hopeful strategy to overcome the global dependence on fossil fuels because it allows for the storage of solar energy and simultaneous mitigation of CO2 emissions. Here, we present a noble metal and Cd-free photocatalyst system for CO2 reduction in water. Ligand-free ZnSe quantum dots (QDs) are used as a visible-light photosensitiser and combined with a phosphonic acid-functionalised Ni(cyclam) catalyst, NiCycP. This hybrid assembly exhibits high activity towards CO2 to CO reduction (Ni-based TON CO > 120), whereas a freely diffusing (anchor-free) catalyst, Ni(cyclam), evolves significantly less CO. Surface modification of ZnSe QDs with 2-mercapto-ethyl dimethylammonium chloride (MEDA) partly suppresses H2 production and increases CO evolution leading to a TONNi CO of > 280 and 33% CO-selectivity after 20 h of visible light irradiation (λ > 400 nm, AM 1.5G, 1 sun). The external quantum efficiency was determined to be 3.4 ± 0.3 % under 400 nm monochromatic light irradiation. Ultrafast transient absorption spectroscopy rationalises the high photocatalytic activity of this catalyst. Band-gap excitation of ZnSe QDs is followed by rapid hole scavenging through the sacrificial electron donor. Excited electrons are subsequently trapped below the ZnSe conduction band which enables efficient charger transfer to NiCycP on the ps time scale. In conclusion, we present ZnSe QDs as promising material for the generation of solar fuels.1
This work was supported by the Christian Doppler Research Association (Austrian Federal Ministry of Science, Research and Economy and the National Foundation for Research, Technology and Development) and the OMV Group.
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