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Stabilization of Pd3−xIn1+x polymorphs with Pd-like crystal structure and their superior performance as catalysts for semi-hydrogenation of alkynes

Johnston, Shaun K; Bryant, Thomas A; Strong, Jonathan; Lazzarini, Laura; Ibhadon, Alex O; Francesconi, M. Grazia

Authors

Shaun K Johnston

Thomas A Bryant

Jonathan Strong

Laura Lazzarini

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Dr Alex Ibhadon A.O.Ibhadon@hull.ac.uk
Reader in Catalysis and Reactor Engineering



Abstract

Selective hydrogenation (semi-hydrogenation) reactions of alkynes rely on Pd-based catalysts to provide the correct pathway to favour formation of double bonds and avoid full hydrogenation to single bonds. Here, we present the preparation and characterisation of "Pd3In"/TiO2 nanocatalysts, which show improved activity and selectivity compared to pure Pd catalysts, towards the liquid phase semi-hydrogenation of 2-methyl-3-butyn-2-ol (MBY) to 2-methyl-3-buten-2-ol (MBE), a fundamental step in the preparation of pharmaceuticals, and other industrially produced substances, as well as a model reaction for the semi-hydrogenation of alkynes. For both the supported and unsupported "Pd3In" alloys (later redefined as Pd3-xIn1+x), we stabilised two new cubic polymorphs with a Pd-like structure, instead of the tetragonal structure as reported so far in the literature. The stabilisation of these new polymorphs was made possible by using a solution-based synthesis and, thanks to the use of different solvents, the reaction was 2 carried out at different temperatures and the Pd/In ratio could be tuned. The same synthetic approach was adapted to prepare two "Pd3In"/TiO2 catalysts by adding the TiO2 support to the reaction mixture, in a practical one-step, one-pot reaction. HREM and X-Ray maps show that the cubic crystal structure of "Pd3In" is maintained when prepared in the presence of the support, however, the support seems to influence the Pd/In ratio.

Citation

Johnston, S. K., Bryant, T. A., Strong, J., Lazzarini, L., Ibhadon, A. O., & Francesconi, M. G. (2019). Stabilization of Pd3−xIn1+x polymorphs with Pd-like crystal structure and their superior performance as catalysts for semi-hydrogenation of alkynes. ChemCatChem, 11(12), 2909-2918. https://doi.org/10.1002/cctc.201900391

Journal Article Type Article
Acceptance Date Apr 17, 2019
Online Publication Date Apr 26, 2019
Publication Date Jun 19, 2019
Deposit Date Apr 30, 2019
Publicly Available Date Apr 27, 2020
Journal ChemCatChem
Print ISSN 1867-3880
Electronic ISSN 1867-3899
Publisher Wiley
Peer Reviewed Peer Reviewed
Volume 11
Issue 12
Pages 2909-2918
DOI https://doi.org/10.1002/cctc.201900391
Keywords Semi-hydrogenation; Nanoalloys; Pd3in
Public URL https://hull-repository.worktribe.com/output/1681749
Publisher URL https://onlinelibrary.wiley.com/doi/10.1002/cctc.201900391
Additional Information This is the accepted manuscript of an article published in ChemCatChem, 2019. The version of record is available at the DOI link in this record.

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