Journal of Aerosol Science, Vol.128, 50-61, 2019
Aerosol synthesis of germanium nanoparticles supported by external seeding: Theoretical and experimental analysis
In this work we present a detailed study of the effect of heterogeneous nucleation on the formation of germanium nanoparticles (Ge NPs) produced from monogermane (GeH4) in a hot wall reactor gas phase synthesis. As external seeding unit we use a hot wire generator (HWG) which produces a stable concentration of aerosol particles. The particle concentration and size of the seeds is easily controllable via the applied voltage and used metal. We demonstrate the importance of seed particles for the production of narrowly distributed Ge NPs with geometrical standard deviations (GSD) < 1.1 in our setup. Thereby, molybdenum and tungsten as wire metal show the best seeding results. The size of the final Ge NPs can be precisely controlled in the range of 20-60 nm. The expansion of Ge lattice seen in XRD and tiny amount of Mo probed by high-resolution STEM-EDXS analysis indicate that the Mo seed particles are most likely dissolved and incorporated in the Ge lattice during growth. Furthermore, we demonstrate an approach to investigate the effect of heterogeneous nucleation on the particle formation by population balance modeling. The results are in good agreement with experimental data. The seed concentration is the key parameter and has a major influence on the nucleation rate.
Keywords:Gas phase synthesis;Germanium;Nanoparticles;Hot wire generator;Heterogeneous nucleation;Simulation