Direct Observation of Morphological and Chemical Changes During the Oxidation of Model Inorganic Ligand-Capped Particles

Functionalization and volatilization are competing reactions during the oxidation of carbonaceous materials and are important processes in many different areas of science and technology. Here we present a combined ambient pressure X-ray photoelectron spectroscopy (APXPS) and grazing incidence X-ray...

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Bibliographic Details
Published inarXiv.org
Main Authors Jaugstetter, Maximilian, Xiao, Qi, Chan, Emory, Salmeron, Miquel, Wilson, Kevin R, Nemšák, Slavomír, Bluhm, Hendrik
Format Paper
LanguageEnglish
Published Ithaca Cornell University Library, arXiv.org 30.06.2024
Subjects
Carbonaceous materials
Functional groups
Ionizing radiation
Ligands
Morphology
Nanoparticles
Oleic acid
Oxidation
Photoelectrons
Pressure
Silicon substrates
Vapor phases
Vaporization
X ray photoelectron spectroscopy
X-ray scattering
X-rays
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Summary:Functionalization and volatilization are competing reactions during the oxidation of carbonaceous materials and are important processes in many different areas of science and technology. Here we present a combined ambient pressure X-ray photoelectron spectroscopy (APXPS) and grazing incidence X-ray scattering (GIXS) investigation of the oxidation of oleic acid ligands surrounding NaYF4 nanoparticles (NPs) deposited onto SiOx/Si substrates. While APXPS monitors the evolution of the oxidation products, GIXS provides insight into the morphology of the ligands and particles before and after the oxidation. Our investigation shows that the oxidation of the oleic acid ligands proceeds at O2 partial pressures of below 1 mbar in the presence of X-rays, with the oxidation eventually reaching a steady state in which mainly CHx and -COOH functional groups are observed. The scattering data reveal that the oxidation and volatilization reaction proceeds preferentially on the side of the particle facing the gas phase, leading to the formation of a chemically and morphologically asymmetric ligand layer. This comprehensive picture of the oxidation process could only be obtained by combining the X-ray scattering and APXPS data. The investigation presented here lays the foundation for further studies of the stability of NP layers in the presence of reactive trace gasses and ionizing radiation, and for other nanoscale systems where chemical and morphological changes happen simultaneously and cannot be understood in isolation.
ISSN:2331-8422