RT journal article
T1 An AI-Powered Methodology for Atomic-Scale Analysis of Heterogenized Correlated Single-Atom Catalysts
A1 Aniceto-Ocaña, Paula
A1 Marqueses Rodríguez, José
A1 Muñoz Ocaña, Juan Manuel
A1 Fernández-Trujillo Rey, María Jesús
A1 García Algarra, Andrés
A1 Rodríguez Chía, Antonio Manuel
A1 Calvino Gámez, José Juan
A1 Castillo González, Carmen Esther
A1 López Haro, Miguel
A2 Ciencia de los Materiales e Ingeniería Metalúrgica y Química Inorgánica
A2 Estadística e Investigación Operativa
K1 aberration corrected HAADF-STEM
K1 catalysis
K1 deep Learning
K1 single atoms
AB Correlated single-atom catalysts offer transformative potential in catalysis, particularly in the field of electrocatalysis, with a focus on oxygen evolution reactions. Advanced characterization is critical to understanding their atomic-scale properties when techniques usually used in molecular science (Nuclear Magnetic Resonance (NMR), X-ray Diffraction (XRD), Infrared spectroscopy (IR), or Mass Spectrometry (MS)) cannot be applied after dispersing them on a carrier material. Here, a methodology that combines machine learning and mathematical optimization techniques to detect and quantify metal–metal interactions within heterobinuclear Au(III)-Pd(II) macrocyclic complexes on atomically resolved high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) images is introduced. Both supervised and unsupervised machine learning methods are evaluated, with the U-net architecture demonstrating superior performance in distinguishing the two involved chemical species. Mathematical optimization models further enhance the reliability of metal pair identification by providing precise distance metrics for the pairs. This methodology allows for the study of both the dynamics and bond interaction of heterobinuclear Au(III)-Pd(II) complexes. Notably, the analysis of time series of images reveals that most metal pairs remained stable under the high-energy electron beam irradiation conditions. Likewise, the Au–Pd distance within the pairs remains unchanged, indicating a robust interaction of the two metals with the ligand even after being deposited on the amorphous carbon substrate.
PB John Wiley and Sons Inc
SN 2366-9608
YR 2025
FD 2025
LK http://hdl.handle.net/10498/38662
UL http://hdl.handle.net/10498/38662
LA eng
DS Repositorio Institucional de la Universidad de Cádiz
RD 08-nov-2026