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Register a new userOxynitride Thin Films versus Particle-Based Photoanodes: a Comparative Study for Photoelectrochemical Solar Water Splitting
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The solar water splitting process assisted by semiconductor photocatalysts attracts growing research interests worldwide for the production of hydrogen as a clean and sustainable energy carrier. Due to their optical and electrical properties several oxynitride materials show great promise for the fabrication of efficient photocatalysts for solar water splitting. This study reports a comparative investigation of particle- and thin films-based photocatalysts using three different oxynitride materials. The absolute comparison of the photoelectrochemical activities favors the particle-based electrodes due to the better absorption properties and larger electrochemical surface area. However, thin films surpass the particle-based photoelectrodes due to their more suitable morphological features that improve the separation and mobility of the photo-generated charge carriers. Our analysis identifies what specific insights into the properties of materials can be achieved with the two complementary approaches.
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Perovskite yttrium tantalum oxynitride is theoretically proposed as a promising semiconductor for solar water splitting because of the predicted bandgap and energy positions of band edges. In experiment, however, we show here that depending on processing parameters, yttrium tantalum oxynitrides exist in multiphases, including the desired perovskite YTaON2, defect fluorite YTa(O,N,o)4, and N-doped YTaO4. These multiphases have bandgaps ranging between 2.13 and 2.31 eV, all responsive to visible light. The N-doped YTaO4, perovskite main phase, and fluorite main phase derived from crystalline fergusonite oxide precursors exhibit interesting photoelectrochemical performances for water oxidation, while the defect fluorite derived from low crystallized scheelite-type oxide precursors show negligible activity. Preliminarily measurements show that loading IrOx cocatalyst on N-doped YTaO4 significantly improves its photoelectrochemical performance encouraging further studies to optimize this new material for solar fuel production.
Photoelectrochemical solar water splitting is a promising approach to convert solar energy into sustainable hydrogen fuel using semiconductor electrodes. Due to their visible light absorption properties, oxynitrides have shown to be attractive photocatalysts for this application. In this study, the influence of the preparation method of CaNbO2N particles on their morphological and optical properties, and thereby their photoelectrochemical performance, is investigated. The best performing CaNbO2N photoanode is produced by ammonolysis of Nb enriched calcium niobium oxide. The enhanced photoactivity arises from an enlarged surface area and superior visible light absorption properties. The photoactivity of this photoanode was further enhanced by photodeposition of Co-Pi co-catalyst and by atomic layer deposition of an Al2O3 overlayer. A photocurrent density of 70 microA.cm-2 at 1.23 V vs RHE was achieved. The observed enhancement of the photoelectrochemical performance after Co-Pi/Al2O3 deposition is the combined effect of the improved kinetics of oxygen evolution due to the Co-Pi co-catalyst and the reduced surface recombination of the photogenerated carriers at the Al2O3 surface layer.
Optimising the photoelectrochemical performance of hematite photoanodes for solar water splitting requires better understanding of the relationships between dopant distribution, structural defects and photoelectrochemical properties. Here, we use complementary characterisation techniques including electron microscopy, conductive atomic force microscopy (CAFM), Rutherford backscattering spectroscopy (RBS), atom probe tomography (APT) and intensity modulated photocurrent spectroscopy (IMPS) to study this correlation in Ti-doped (1 cat.%) hematite films deposited by pulsed laser deposition (PLD) on F:SnO2 (FTO) coated glass substrates. The deposition was carried out at 300 {deg}C, followed by annealing at 500 deg C for 2 h. Upon annealing, Ti was observed by APT to segregate to the hematite/FTO interface and into some hematite grains. Since no other pronounced changes in microstructure and chemical composition were observed by electron microscopy and RBS after annealing, the non-uniform Ti redistribution seems to be the reason for a reduced interfacial recombination in the annealed films, as observed by IMPS. This results in a lower onset potential, higher photocurrent and larger fill factor with respect to the as-deposited state. This work provides atomic-scale insights into the microscopic inhomogeneity in Ti-doped hematite thin films and the role of defect segregation in their electrical and photoelectrochemical properties.
In recent years, hematite potential as a photoanode material for solar hydrogen production has ignited a renewed interest in its physical and interfacial properties, which continues to be an active field of research. Research on hematite photoanodes provides new insights on the correlations between electronic structure, transport properties, excited state dynamics and charge transfer phenomena, and expands our knowledge on solar cell materials into correlated electron systems. This research news article presents a snapshot of selected theoretical and experimental developments linking the electronic structure to the photoelectrochemical performance, with particular focus on optoelectronic properties and charge carrier dynamics.
The oxygen evolution reaction (OER) at the surface of semiconductor photoanodes involves photo-generated holes that oxidize water. A certain fraction of the holes that reach the surface recombine with electrons from the conduction band, giving rise to the surface recombination loss. The charge transfer efficiency, xt, defined as the ratio between the flux of holes that contribute to the water oxidation reaction and the total flux of holes that reach the surface, is an important parameter that helps to distinguish between bulk and surface recombination losses. However, accurate determination of xt by conventional voltammetry measurements is complicated because only the total current is measured and it is difficult to discern between different contributions to the current. Chopped light measurement and hole scavenger measurement techniques are widely employed to determine xt, but they often lead to errors. Intensity modulated photocurrent spectroscopy (IMPS) is better suited for accurate determination of xt because it provides direct information on both the total photocurrent and the surface recombination current. Careful analysis of IMPS measurements at different light intensities is required to account for nonlinear effects. We compare the xt values obtained by these methods using heteroepitaxial hematite photoanodes. A wide spread of xt values is obtained by different analysis methods and different light sources and light intensities. Statistical analysis of the results show good correlation between different methods for measurements carried out with the same light source, light intensity and potential. However, there is a considerable spread in the results obtained by different methods. For accurate determination of xt, we recommend IMPS measurements with a bias light intensity such that the irradiance is as close as possible to the standard solar spectrum.
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