The catalytic properties of nanoparticles depend on their size, shape and surface/defect structure, with the entire catalyst performance being governed by the corresponding distributions. Herein, we present two routes of mono- and bimetallic nanoparticle synthesis that enable control of the structural parameters, i.e., wet-chemical synthesis and laser ablation in liquid-phase. The latter is particularly suited to create defect-rich nanoparticles. Impregnation routes were applied to prepare Ni and NiCu nanoparticles, whereas nano- and femtosecond laser ablation in liquid-phase were employed to prepare Ni and NiAu nanoparticles. The effects of the Ni:Cu ratio in impregnation and of laser fluence and liquid-medium on laser ablation are discussed. The atomic structure and (surface) composition of the nanoparticles were characterized by electron microscopic (BF-TEM, DF-TEM, HRTEM) and spectroscopic/diffraction techniques (EDX, SAED, XPS, IR), complemented by theory (DFT). The chemically synthesized bimetallic NiCu nanoparticles initially had Cu-rich surfaces, which changed to Ni-rich upon reaction. For laser ablation, depending on conditions (fluence, type of liquid), highly defective, ordered, or core/shell-like nanoparticles were produced. The case studies highlight the specific benefits of each preparation method for catalyst synthesis and discuss the potential of nanoparticles produced by pulsed laser ablation for catalytic applications.

Adding photocatalytically active TiO₂ nanoparticles (NPs) to polymeric paints is a feasible route toward self-cleaning coatings. While paint modification by TiO₂-NPs may improve photoactivity, it may also cause polymer degradation and release of toxic volatile organic compounds. To counterbalance adverse effects, a synthesis method for nonmetal (P, N, and C)-doped TiO₂-NPs is introduced, based purely on waste valorization. PNC-doped TiO₂-NP characterization by vibrational and photoelectron spectroscopy, electron microscopy, diffraction, and thermal analysis suggests that TiO₂-NPs were modified with phosphate (P=O), imine species (R=N-R), and carbon, which also hindered the anatase/rutile phase transformation, even upon 700 °C calcination. When added to water-based paints, PNC-doped TiO₂-NPs achieved 96% removal of surface-adsorbed pollutants under natural sunlight or UV, paralleled by stability of the paint formulation, as confirmed by micro-Fourier transform infrared (FTIR) surface analysis. The origin of the photoinduced self-cleaning properties was rationalized by three-dimensional (3D) and synchronous photoluminescence spectroscopy, indicating that the dopants led to 7.3 times stronger inhibition of photoinduced e^-/h⁺ recombination when compared to a benchmark P25 photocatalyst.

Homogeneous polycrystalline Fe_xO_y nanoparticles were generated by ablation of iron targets in water by nanosecond laser pulses at 532 nm. In ethanol, crystalline core‐shell Fe/Fe_xO_y structures with size medians around 20 nm were produced. The ablation of FeW_xO_y targets in water resulted in crystalline hollow shells and homogeneous FeW_xO_y nanoparticles. In contrast, amorphous core‐shell FeW_xO_y nanoparticles with a median size of 17 nm were produced in ethanol. The size distribution of both the Fe_xO_y and the FeW_xO_y particles showed a slight dependence on fluence and pulse number. This may be related to primary and secondary ablation and modification mechanisms.

Nanocrystalline silicon nanoparticles with a median crystallite size of 3–4 nm and several crystalline phases and defects (e.g. twin boundary) were produced by femtosecond laser processing of a SiO₂/Si target in various organic fluids. Furthermore, a nanoscaled amorphous oxide layer and a few atomic layers of a graphite shell were detected in ethanol and 2-butanol correspondingly. The ultrafast laser pulses may manipulate nanostructures at the atomic level and generate a high density of defects; this may be correlated with significant thermal stresses on nanoparticles and rapid condensation of primary nanoparticles with high cooling rates. Size distribution width and a polydispersity index slightly increased with increasing laser fluence in ethanol. In 2-butanol, the maximum ablation volume was observed. The specific ablation rates in 2-butanol and ethanol were approximately five times higher than n-hexane. The lowest ablation efficiency in n-hexane can be associated with femtosecond laser-induced photolysis and pyrolysis of solvent molecules, as total energy deposition on the material may be reduced due to the formation of carbonaceous products. The roughened zones (average roughness of ∼400 nm) in circumferences of the ablated craters in 2-butanol may be related to a correlation between the erosive power of the vapour bubble collapse and higher pressure at the bubble wall in relatively high dynamic viscosity fluids. Furthermore, sputtering of a pristine surface by releasing nanoparticles from the collective collapse of up-flow vapour bubbles can also contribute to the generation of roughened regions.