Publication date: 15th December 2025
Hydrogen is a zero-emission energy carrier, yet its global production remains dominated by fossil fuels. With the accelerating impacts of climate change, the transition to renewable energy sources has become critical to achieving the United Nations Sustainable Development Goal 7: Affordable and Clean Energy. Semiconductor-based artificial photosynthesis, inspired by natural photosynthetic systems, represents a promising route to generate green hydrogen through solar-driven water splitting. To improve solar energy conversion efficiency, controlling crystal morphology and crystal defects, and elucidating their effect on properties are crucial. Mixed-anion compounds have emerged as promising photocatalysts [1]. Within this class of materials, BaTaO2N stands out as a visible-light-responsive photocatalyst (~600 nm) because of its small bandgap (Eg = 1.8 eV), suitable band edge positions for visible-light-induced water splitting, chemical stability, and nontoxicity [2,3]. Conventionally synthesized via a two-step oxide precursor and high-temperature nitridation route, BaTaO2N crystals often suffer from defect formation, which is detrimental to their photocatalytic activity. In this work, we applied an NH3-assisted direct flux growth method to reduce defect density, tune the bandgap via cation doping, and investigate the influence of morphology, size, and porosity on photocatalytic and photoelectrochemical performance of BaTaO2N crystals. The findings demonstrate that the BaTaO2N crystals grown directly by NH3-assited KCL flux method have less defect density and BaTaO2N crystals synthesized by two-step method without KCl flux exhibit higher surface areas and enhanced photocurrents due to increased active sites facilitating efficient CoOx cocatalyst dispersion. Furthermore, we also explored the impact of crystal shape and size on the property and photocatalytic activity of β-TaON and Ta3N5.
This work was funded by a Novo Nordisk Foundation Grant (NNF23OC0079059).
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