RT Journal Article
T1 Quantitative, Spectro-kinetic Analysis of Oxygen in Electron-Beam Sensitive, Multimetallic Oxide Nanostructures
A1 López-Haro, Miguel
A1 Gómez Recio, Isabel
A1 Pan, Huiyan
A1 Delgado, Juan
A1 Chen, Xiaowei
A1 Cauqui, Miguel
A1 Pérez-Omil, José
A1 Ruiz González, María Luisa
A1 Hernando González, María
A1 Parras Vázquez, Marina Marta
A1 González Calbet, José María
A1 Calvino, José
AB The oxygen stoichiometry of hollandite, KxMnO2-δ, nanorods has been accurately determined from a quantitative analysis of scanning-transmission electron microscopy (STEM) X-Ray Energy Dispersive Spectroscopy (XEDS) experiments carried out in chrono-spectroscopy mode. A methodology combining 3D reconstructions of high-angle annular dark field electron tomography experiments, using compressed-sensing algorithms, and quantification through the so-called ζ-factors method of XEDS spectra recorded on a high-sensitivity detector has been devised to determine the time evolution of the oxygen content of nanostructures of electron-beam sensitive oxides. Kinetic modeling of O-stoichiometry data provided K0.13MnO1.98 as overall composition for nanorods of the hollandite. The quantitative agreement, within a 1% mol error, observed with results obtained by macroscopic techniques (temperature-programmed reduction and neutron diffraction) validate the proposed methodology for the quantitative analysis, at the nanoscale, of light elements, as it is the case of oxygen, in the presence of heavy ones (K, Mn) in the highly compromised case of nanostructured materials which are prone to electron-beam reduction. Moreover, quantitative comparison of oxygen evolution data measured at macroscopic and nanoscopic levels allowed us to rationalize beam damage effects in structural terms and clarify the exact nature of the different steps involved in the reduction of these oxides with hydrogen.
PB Oxford University Press
SN 1431-9276
YR 2023
FD 2023
LK https://hdl.handle.net/20.500.14352/91874
UL https://hdl.handle.net/20.500.14352/91874
LA eng
NO López-Haro M, Gómez-Recio I, Pan H, Delgado JJ, Chen X, Cauqui MA, Pérez-Omil JA, Ruiz-González ML, Hernando M, Parras M, González-Calbet JM, Calvino JJ. Quantitative, Spectro-kinetic Analysis of Oxygen in Electron-Beam Sensitive, Multimetallic Oxide Nanostructures. Microsc Microanal. 2023 Jun 9;29(3):900-912. doi: 10.1093/micmic/ozad037. PMID: 37749688.
NO Junta de Andalucía
NO Ministerio de Ciencia e Innovación (España)
DS Docta Complutense
RD 6 abr 2025