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Entirely Self-organized: Arrayed Single-Particle-in-a-Cavity Reactors for Highly Efficient and Selective Catalytic/Photocatalytic Energy Conversion and Solar Light Reaction Engineering

Final Report Summary - APHOTOREACTOR (Entirely Self-organized: Arrayed Single-Particle-in-a-Cavity Reactors for Highly Efficient and Selective Catalytic/Photocatalytic Energy Conversion and Solar Light Reaction Engineering)

The project dealt with a series of overlaid self-organization processes that enabled the creation of nanostructured photocatalytic platforms with unprecedented properties in terms of reactivity control.
For this, a series of self-assembly tools on the mesoscale were developed to create highly uniform arrays of single-catalyst-particle-in-a-single-oxide-cavity. We proved such nanostructuring pathways to accomplish a 100% reliable placement of a single catalyst particles in nm sized cavities. This enabled catalytic features of noble metal nanoparticles, e.g. Pt, Au etc., and also non noble elements, to interact with the semiconductive, photocatalytic properties of a Ti oxide cavities.
The cavities were optimized for optical and electronic properties by doping or via lattice defect or band-gap engineering. Tuning the geometric dimensions to the range of a few nm not only allowed for taking benefit from a maximized carrier transfer efficiency from-oxide-to-particle but also to reach high metal particle surfaces for a dramatically enhanced activity per loaded catalyst mass.
Catalyst reactivity and economy were improved via alloying effects with earth abundant elements, this increasing at the same time also the tolerance against deactivation and poisoning, or through dealloying principles to maximize the active metal catalyst surface and density of reaction sites. In addition, the precise nanoscopic design led to anti-aggregation catalyst/support assemblies with substantially enhanced catalyst life-time, and at a reduced cost.
Overall, the project yielded novel, highly precise combined catalyst/photocatalyst assemblies for photocatalytic applications such as direct water splitting, oxidation/mineralization reactions (pollutant degradation) and photocatalytic organic synthesis. Such combined catalytic/photocatalytic pathways enabled such reactions to be carried out ecologically, namely under solar light illumination, and economically, i.e. with drastically enhanced efficiency and selectivity.
The nanoscopic design developed yielded a radical change in the controllability of length and time-scales (reactant, charge carrier and ionic transport in the substrate) in combined photocatalytic/catalytic reactions.
The nanoscale assembly principles explored in this project were optimized towards scalability to allow to create in future research square meters of nanoscopically ordered catalyst surfaces, for implementation of such nanoscale principles, approaches and concepts in industrial scale reactors and applications.