期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 37, 页码 20407-20416出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202103641
关键词
bismuth; in situ studies; nanostructures; pair distribution function; small-angle X-ray scattering
资金
- European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme [804066]
- Danish Agency for Science and Higher Education
- Deutsche Forschungsgemeinschaft [DFG SPP1415, ME 2284/3-2]
- Innovation Fund Denmark (IFD) [5152-00005B]
- Projekt DEAL
- Siemens Foundation
- European Research Council (ERC) [804066] Funding Source: European Research Council (ERC)
The study demonstrates the formation mechanism of metal oxido nanoclusters with a [Bi38O45] core using a combination of in situ pair distribution function (PDF) analysis and small-angle X-ray scattering (SAXS). The identification of [Bi22O26] as an intermediate species highlights the power of combined PDF and SAXS analysis for insights into nucleation on an atomic scale. Furthermore, the study shows how the interaction between nanoclusters and solvent is influenced by the nature of the ligands on the cluster surface.
The combination of in situ pair distribution function (PDF) analysis and small-angle X-ray scattering (SAXS) enables analysis of the formation mechanism of metal oxido nanoclusters and cluster-solvent interactions as they take place. Herein, we demonstrate the method for the formation of clusters with a [Bi38O45] core. Upon dissolution of crystalline [Bi6O5(OH)(3)(NO3)(5)]center dot 3H(2)O in DMSO, an intermediate rapidly forms, which slowly grows to stable [Bi38O45] clusters. To identify the intermediate, we developed an automated modeling method, where smaller [BixOy] structures based on the [Bi38O45] framework are tested against the data. [Bi22O26] was identified as the main intermediate species, illustrating how combined PDF and SAXS analysis is a powerful tool to gain insight into nucleation on an atomic scale. PDF also provides information on the interaction between nanoclusters and solvent, which is shown to depend on the nature of the ligands on the cluster surface.
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