1. All-in-one visible-light-driven water splitting by combining nanoparticulate and molecular co-catalysts on CdS nanorods
- Author
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Michael T. Carlson, Frank Würthner, Christian M. Wolff, Panajotis Livadas, Jochen Feldmann, Peter D. Frischmann, Jacek K. Stolarczyk, Robin Wein, Frank Jäckel, Marcus Schulze, and Bernhard J. Bohn
- Subjects
Materials science ,Hydrogen ,Renewable Energy, Sustainability and the Environment ,Energy Engineering and Power Technology ,chemistry.chemical_element ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Redox ,0104 chemical sciences ,Electronic, Optical and Magnetic Materials ,Catalysis ,Fuel Technology ,Chemical engineering ,chemistry ,Nanocrystal ,ddc:540 ,Institut für Chemie ,Water splitting ,Nanorod ,0210 nano-technology ,Photocatalytic water splitting ,Visible spectrum - Abstract
Full water splitting into hydrogen and oxygen on semiconductor nanocrystals is a challenging task; overpotentials must be overcome for both half-reactions and different catalytic sites are needed to facilitate them. Additionally, efficient charge separation and prevention of back reactions are necessary. Here, we report simultaneous H-2 and O-2 evolution by CdS nanorods decorated with nanoparticulate reduction and molecular oxidation co-catalysts. The process proceeds entirely without sacrificial agents and relies on the nanorod morphology of CdS to spatially separate the reduction and oxidation sites. Hydrogen is generated on Pt nanoparticles grown at the nanorod tips, while Ru(tpy)(bpy)Cl-2-based oxidation catalysts are anchored through dithiocarbamate bonds onto the sides of the nanorod. O-2 generation from water was verified by O-18 isotope labelling experiments, and time-resolved spectroscopic results confirmed efficient charge separation and ultrafast electron and hole transfer to the reaction sites. The system demonstrates that combining nanoparticulate and molecular catalysts on anisotropic nanocrystals provides an effective pathway for visible-light-driven photocatalytic water splitting.
- Published
- 2018