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Subnanometer Substructures in Nanoassemblies Formed from Clusters under a Reactive Atmosphere Revealed Using Machine Learning

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journal contribution
posted on 26.08.2018, 00:00 by Janis Timoshenko, Avik Halder, Bing Yang, Soenke Seifert, Michael J. Pellin, Stefan Vajda, Anatoly I. Frenkel
Size-selected clusters, soft-landed on an oxide substrate, is a promising and highly tunable material for heterogeneous catalysis. Agglomeration of the deposited clusters, however, leads to changes in the particle properties and structure. The latter for such cluster assemblies can also be different from that in self-standing nanoparticles of similar sizes. To monitor the formation of such complex materials, in situ studies at different length scales are required. Toward that goal, we combined small-angle X-ray scattering (SAXS), X-ray absorption near-edge structure (XANES) spectroscopy, ab initio simulations, and machine learning (artificial neural network) techniques. We detected significant differences between the sizes of particle agglomerates, as probed by SAXS, and the sizes of locally ordered regions, as seen by XANES. We interpret these differences as an evidence for the fractal, grape-cluster-like structure of the agglomerates; thus, XANES and SAXS provide highly complementary structural information. This finding can have a profound effect on our understanding of particle sintering and assembly processes and of structure–properties relationship in ultradispersed metal catalysts in reaction conditions.

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