RESUMEN
The unprecedented impact of human activity on Earth's climate and the ongoing increase in global energy demand have made the development of carbon-neutral energy sources ever more important. Hydrogen is an attractive and versatile energy carrier (and important and widely used chemical) obtainable from water through photocatalysis using sunlight, and through electrolysis driven by solar or wind energy1,2. The most efficient solar hydrogen production schemes, which couple solar cells to electrolysis systems, reach solar-to-hydrogen (STH) energy conversion efficiencies of 30% at a laboratory scale3. Photocatalytic water splitting reaches notably lower conversion efficiencies of only around 1%, but the system design is much simpler and cheaper and more amenable to scale-up1,2-provided the moist, stoichiometric hydrogen and oxygen product mixture can be handled safely in a field environment and the hydrogen recovered. Extending our earlier demonstration of a 1-m2 panel reactor system based on a modified, aluminium-doped strontium titanate particulate photocatalyst4, we here report safe operation of a 100-m2 array of panel reactors over several months with autonomous recovery of hydrogen from the moist gas product mixture using a commercial polyimide membrane5. The system, optimized for safety and durability, and remaining undamaged on intentional ignition of recovered hydrogen, reaches a maximum STH of 0.76%. While the hydrogen production is inefficient and energy negative overall, our findings demonstrate that safe, large-scale photocatalytic water splitting, and gas collection and separation are possible. To make the technology economically viable and practically useful, essential next steps are reactor and process optimization to substantially reduce costs and improve STH efficiency, photocatalyst stability and gas separation efficiency.
RESUMEN
Various types of Z-scheme systems for water splitting under visible light irradiation were successfully developed by employing Rh- and Ir-doped metal oxide powdered materials with relatively narrow energy gaps (EG): BaTa2O6:Ir,La (EG: 1.9-2.0 eV), NaTaO3:Ir,La (EG: 2.1-2.3 eV), SrTiO3:Ir (EG: 1.6-1.8 eV), NaNbO3:Rh,Ba (EG: 2.5 eV) and TiO2:Rh,Sb (EG: 2.1 eV), with conventional SrTiO3:Rh (an H2-evolving photocatalyst) or BiVO4 (an O2-evolving photocatalyst), and suitable electron mediators. The Z-scheme systems were classified into three groups depending on the combination of H2- and O2-evolving photocatalysts and electron mediator. The Z-scheme systems combining BaTa2O6:Ir,La with BiVO4, and NaTaO3:Ir,La with BiVO4 were active when a [Co(bpy)3]3+/2+ redox couple was used rather than an Fe3+/2+ one. The combination of SrTiO3:Ir with SrTiO3:Rh gave an activity when the [Co(bpy)3]3+/2+ and Fe3+/2+ redox couple ionic mediators were used. The Z-scheme systems combining NaNbO3:Rh,Ba and TiO2:Rh,Sb with SrTiO3:Rh showed activities by using the [Co(bpy)3]3+/2+ and Fe3+/2+ redox couples and also via interparticle electron transfer by just contact with/without reduced graphene oxide (RGO). These suitable combinations can be explained based on the impurity levels of doped Rh3+ and Ir3+ toward the redox potentials of the ionic mediators for the Z-scheme systems employing ionic mediators, and p-/n-type and onset potentials of the photocurrent in the photoelectrochemical properties of those photocatalyst materials for the Z-scheme systems working via interparticle electron transfer.
RESUMEN
SnNb2O6 has arisen as a candidate for photoanodes for solar water splitting. CoOx cocatalyst-loaded SnNb2O6 showed a stable, high anodic photocurrent with an incident photon-to-current conversion efficiency (IPCE) of 18% at 0.6 VRHE and a half-cell solar-to-hydrogen (HC-STH) efficiency of 0.39% at 0.6 VRHE.