Single Copper Nanoparticle Oxidation
Licentiate thesis, 2019
Since only a handful of single particle studies concerning the oxidation of Cu nanoparticles exist to date, all but one by means of transmission electron microscopy (TEM), in this thesis I have developed an in situexperimental method for studying the oxidation of single Cu nanoparticles. It combines the structural information from TEM imaging with a non-invasive optical dark-field scattering spectroscopy method – plasmonic nanospectroscopy – that enables the tracking of oxidation kinetics in real time. In this way, I can minimize exposure of the particles to the electron beam in the TEM, and thus minimize the risk for beam-induced structural and chemical changes to the particles during the experiments.
Using this platform in combination with finite-difference time-domain electrodynamics simulations of models representing different stages during the oxidation, I was able to systematically analyze the single particle optical response measured in the experiments and thus shed light on the oxidation of the single Cu nanoparticles from a mechanistic perspective. As the first key result, we found a distinct evolution of the single particle dark-field scattering spectra of single Cu nanoparticles indicative of Kirkendall void formation. As the second key result, we identified a clear dependence of the induction time to the onset of Kirkendall void formation on the grain structure of the single nanoparticles, where an abundance of high-angle grain boundaries favors the coalescence of vacancies into one large void.
dark-field scattering spectroscopy
transmission electron microscopy
nanoscale Kirkendall effect
Chalmers, Physics, Chemical Physics
Nilsson, S., Albinsson, D., Antosiewicz, T., Friztsche, J., Langhammer, C., In situ Plasmonic Nanospectroscopy of Single Cu Nanoparticle Oxidation and Kirkendall Void Formation
Nilsson, S., Albinsson, D., Bastos da Silva Fanta, A., Friztsche, J., Langhammer, C., Grain Boundary Mediated Oxidation of Single Cu Nanoparticles
Single Particle Catalysis in Nanoreactors (SPCN)
Knut and Alice Wallenberg Foundation (KAW2015.0057), 2016-01-01 -- 2020-12-31.
Areas of Advance
Nanoscience and Nanotechnology (SO 2010-2017, EI 2018-)
Chalmers Materials Analysis Laboratory
Opponent: Maria Messing, Lunds Universitet, Sverige