In our work, UV-response with a small visible light absorption TiO2 nanoparticles were supported on lamellar La2NiO4 perovskite to build a type I heterojunction for efficient hydrogen production under visible light. It was found that, with the increase of La2NiO4 contents, the hydrogen production rates gradually increased and amounted to the highest value when the mass fraction of La2NiO4 was 8 wt. %, which is 39.5 times that of the initial La2NiO4 nanosheets without the cocatalyst Pt. When 1 wt. % Pt was loaded, the photocatalytic activity for the composite photocatalyst increased by 369.0 times that of the initial La2NiO4. Our work should be of value for the preparation of visible responsive heterojunction photocatalysts with high activity, fair stability, and low toxicity.
Most of the traditional photocatalytic hydrogen productions were conducted under room temperature. In this work, we selected nonplasmonic Pt metal anchored on TiO2 nanoparticles with photothermal activity to explore more efficient hydrogen production technology over the whole solar spectrum. Photothermal experiments were carried out in a carefully designed top irradiated photocatalytic reactor that can withstand high temperature and relatively higher pressure. Four typical organic materials, i.e., methyl alcohol (MeOH), trielthanolamne (TEOA), formic acid (HCOOH) and glucose, were investigated. Formic acid, a typical hydrogen carrier, was found to show the best activity. In addition, the effects of different basic parameters such as sacrificial agent concentration and the temperature on the activity of hydrogen generation were systematically investigated for understanding the qualitative and quantitative effects of the photothermal catalytic reaction process. The hydrogen yields at 90 °C of the photothermal catalytic reaction with Pt/TiO2 are around 8.1 and 4.2 times higher than those of reactions carried out under photo or thermal conditions alone. We can see that the photothermal hydrogen yield is not the simple sum of the photo and thermal effects. This result indicated that the Pt/TiO2 nanoparticles can efficiently couple photo and thermal energy to more effectively drive hydrogen production. As a result, the excellent ability makes it superior to other conventional semiconductor photocatalysts and thermal catalysts. Future works could concentrate on exploring photothermal catalysis as well as the potential synergism between photo and thermal effects to find more efficient hydrogen production technology using the whole solar spectrum.
When dispersed in water, nanoscale photocatalysts can aggregate into microscale secondary particles due to their high surface energy. The interaction between the incident photons and the aggregated particles is expected to be significantly changed due to their comparable length scales. Hydrodynamics of the particles after aggregation and the resultant photonic flux distributions in slurry photocatalytic reactors are therefore essential. The magnetically stirred photocatalytic reactor is compact and simple for fabrication, and therefore can be readily employed in lab-scale photocatalytic tests. However, studies toward its optimization are rare. In our study, the photocatalyst distribution was simulated using a Eulerian–Lagrangian approach, while the evolution of free liquid surface led by magnetic stirring was modeled by volume of fluid method. Subsequently, based on the photocatalyst distribution, the photonic flux distribution was obtained through a mean free path-based Monte Carlo method. Outcomes suggest that at a stirring speed of 900 rpm, the 10 μm particles can be well suspended, and a moderate free liquid surface will also be present. Moreover, under sufficient stirring, larger catalyst particles are more likely to be densely distributed in the outer region, which contributes to an increase in the overall photonic absorption even higher than the one with evenly distributed photocatalysts.
My research group in the State Key Laboratory of Multiphase Flow in Power Engineering (SKLMF), Xi’an Jiaotong University has been focusing on renewable energy, especially solar hydrogen, for about 20 years. In this presentation, I will present the most recent progress in our group on solar hydrogen production using light and heat. Firstly, “cheap” photoelectrochemical and photocatalytic water splitting, including both nanostructured materials and pilot-scale demonstration in our group for light-driven solar hydrogen (artificial photosynthesis) will be introduced. Then I will make a deep introduction to the achievements on the thermal-driven solar hydrogen, i.e., biomass/coal gasification in supercritical water for large-scale and low-cost hydrogen production using concentrated solar light.
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