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Facile synthesis of precious-metal single-site catalysts using organic solvents

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Single site catalysts can present high activity and selectivity in many catalytic reactions. The synthesis of these materials by impregnation from strongly oxidising aqueous solutions or pH-controlled deposition often leads to low metal loadings or a range of metal species. We have prepared single site catalyts by a  simple impregnation of the metal precursors onto activated carbon from a low boiling point, low polarity solvent, such as acetone, results in catalysts with an atomic dispersion of cationic metal species.

This file contains electron microscopy imaging of the fresh single site catalysts. In all cases the fresh catalyst contains atomically disperesed metal species, mostly containing single atoms but some dimers and small clusters can be seen as well.

These observations for the microscopy study is supported by X-ray absorption spectroscopy studies. This file contains XANES and EXAFS analysis of the fresh catalysts, the EXAFS is showing no metal-metal contributions in all cases. The catalysts are also studied after heating in the reactor under argon to the reaction temperature, after 10 minutes of reaction and after 240 minutes or reaction. EXAFS data shows no metal-metal contributions in any of these steps. 

XRD of all catalyst are included, no reflections from the active metal can be seen in all cases.

The XAS data is supported by XPS data, this shows the presence of acac ligands in the case of the fresh Ru, Pt and Pd catalysts. It also shows that this ligand is replaced by chloride after reaction.

And testing data in the acetylene hydrochlorination reaction is attached. This show the comparison between the Au/C catalyst prepared via this new method and the 'standard' aqua regia catalysts. Next to this the performance of catalysts prepared by a varytiy of solvents is included as well as the Pt, Ru and Pd single site catalysts. 

Research results based upon these data are published at https://doi.org/10.1038/s41557-020-0446-z


Funding

Heterogeneous catalysis using nanomaterials (2016-10-03 - 2020-09-30); Parmentier, Tanja. Funder: Cardiff University

History

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CasaXPS, Origin 9, Athena

Data-collection start date

2018-01-01

Data-collection end date

2020-01-01

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