Publication date: 15th December 2025
The direct conversion of solar energy into chemical energy in the form of solar fuels (e.g. green hydrogen), has the potential to contribute significantly to cover our energy needs [1,2]. Due to its comparably simple setup photoelectrochemical (PEC) water splitting shows promise as a cost-effective method for producing green hydrogen in the future [3,4]. A PEC system consists of two spatially separated electrodes connected via an ohmic contact, with the water oxidation taking place on the anode side and the hydrogen reduction on the cathode side of the cell [5].
While there have been significant advancements regarding the efficiency of PEC systems, their stability remains a major challenge [2,4]. So far, mainly two approaches have been pursued to improve the stability of photoelectrodes. Material-focused strategies (such as protective layers, surface engineering, cocatalysts, and doping) and device-level strategies (such as electrolyte engineering, reactor configuration, and operation conditions) [6, 7, 8, 9]. The best choice between those depends primarily on the design of the photoelectrode and its primary degradation mechanism. For example, in BiVO₄-based photoanodes, where dissolution is the main issue, electrolyte engineering, particularly saturating the electrolyte with V⁵⁺, has proven highly effective in reducing dissolution and thus enhancing photoelectrode stability [10]. Meanwhile for LaTiO₂N (LTON) based photoanodes, where degradation is dominated by cocatalyst related performance loss, stability improvements should focus on increasing cocatalyst stability.
In this study the stability of LTON based photoanodes was improved by tuning cocatalyst deposition. LTON was synthesized via solid state synthesis followed by thermal ammonolysis. The photoanodes were prepared by electrophoretic deposition followed by TiCl4 necking. The cocatalysts were deposited via dip coating in ethanolic Co(NO3)2 and Ni(NO3)2 solutions, followed by annealing at elevated temperatures. To improve their stability the concentration of the solution, the dipping time as well as the annealing time and temperature have been varied. Further the annealing was performed in both oxidative (air) and reductive atmosphere (ammonia) followed by a further annealing step in air. The stability of the photoanodes was evaluated via long time chronoamperometries at 1.23 V vs RHE. Compositional and morphological changes of the photoanodes were investigated using SEM and HREM, while cocatalyst dissolution and electrolyte compositions were determined by ICPMS.
Funding from the Swiss National Science Foundation Sinergia Grant number CRSII5_20225 is gratefully acknowledged. The TEM infrastructure was funded via the infrastructure call BIOMAT-TEM from the Austrian FFG (grant number 37120633). J.Z. was supported via the Interreg project Bayern-Österreich 2021–2027 ReBi (CCI-Nr. 2021TC16RFCB004).
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