Gas-Phase Nitrogen Doping of Monolithic TiO2 Nanoparticle-Based Aerogels for Efficient Visible Light-Driven Photocatalytic H2 Production

The development of visible light-active photocatalysts is essential for increasing the conversion efficiency of solar energy into hydrogen (H₂). Here, we present a facile method for nitrogen doping of monolithic titanium dioxide (TiO₂) nanoparticle-based aerogels to activate them for visible light. Plasma-enhanced chemical vapor deposition at low temperature enables efficient incorporation of nitrogen into preformed TiO₂ aerogels without compromising their advantageous intrinsic characteristics such as large surface area, extensive porosity, and nanoscale properties of the semiconducting building blocks. By balancing the dopant concentration and the defects, the nitridation improves optical absorption and charge separation efficiency. The nitrogen-doped TiO₂ nanoparticle-based aerogels loaded with palladium (Pd) nanoparticles show a significant enhancement in visible light-driven photocatalytic H₂ production (3.1 mmol h^-1 g^-1) with excellent stability over 5 days. With this method, we introduce a powerful tool to tune the properties of nanoparticle-based aerogels after synthesis for a specific application, as exemplified by visible light-driven H₂ production.