Proceedings of nanoGe September Meeting 2017 (NFM17)
Publication date: 20th June 2016
The development of an efficient, cheap and robust water-splitting catalyst remains the bottleneck step to realizing artificial photosynthesis. Materials based on Prussian blue (iron(III)hexacyanoferrate(II)), which fulfill all those criteria, have shown high catalytic activities with exceeding long-term stabilities.
Notwithstanding, the detailed catalytic mechanisms remain unclear. In combining experimental methods with theoretical calculations we want to elucidate the underlying photo-physical mechanisms and its determining factors, such as electronic structure and charge-transfer properties.
For this, catalytic systems were prepared by modifying well-known photo catalytic materials, such as α-Fe2O3 and BiVO4, with cobalt iron analogues of Prussian blue (CoFe-PB, Cox[Fe(CN)6]y). The use of CoFe-PB as a co-catalyst largely increases the photocurrent and significantly lowers the onset potential of light-induced water oxidation. Moreover, it is highly stable over a wide range of pH. We studied the electrochemical behaviour, catalytic efficiency and impedance under light and electrical field conditions. Also transient absorption spectroscopy (TAS) is used to gain more information about the behaviour of the system.
We employed various theoretical simulations based on Density Functional Theory, DFT, and evaluated their applicability. It was found that common DFT methods are insufficient to accurately describe the complex electronic and magnetic structure of Prussian blues and functionals of a higher degree of complexity are needed. With this, we developed a computational approach to investigate these systems. Moreover, we found out new insights about the electronic and magnetic structure, which might be crucial to its photo catalytic applications.
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