Luneau Lab

at Chalmers University of Technology in Gothenburg, Sweden

Achieving High Selectivity for Alkyne Hydrogenation at High Conversions with Compositionally Optimized PdAu Nanoparticle Catalysts in Raspberry Colloid-Templated SiO2


Journal article


M. Luneau, T. Shirman, Alexandre C. Foucher, Kaining Duanmu, David M. A. Verbart, P. Sautet, E. Stach, J. Aizenberg, R. Madix, C. Friend
ACS Catalysis, 2020

Semantic Scholar DOI
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APA   Click to copy
Luneau, M., Shirman, T., Foucher, A. C., Duanmu, K., Verbart, D. M. A., Sautet, P., … Friend, C. (2020). Achieving High Selectivity for Alkyne Hydrogenation at High Conversions with Compositionally Optimized PdAu Nanoparticle Catalysts in Raspberry Colloid-Templated SiO2. ACS Catalysis.


Chicago/Turabian   Click to copy
Luneau, M., T. Shirman, Alexandre C. Foucher, Kaining Duanmu, David M. A. Verbart, P. Sautet, E. Stach, J. Aizenberg, R. Madix, and C. Friend. “Achieving High Selectivity for Alkyne Hydrogenation at High Conversions with Compositionally Optimized PdAu Nanoparticle Catalysts in Raspberry Colloid-Templated SiO2.” ACS Catalysis (2020).


MLA   Click to copy
Luneau, M., et al. “Achieving High Selectivity for Alkyne Hydrogenation at High Conversions with Compositionally Optimized PdAu Nanoparticle Catalysts in Raspberry Colloid-Templated SiO2.” ACS Catalysis, 2020.


BibTeX   Click to copy

@article{m2020a,
  title = {Achieving High Selectivity for Alkyne Hydrogenation at High Conversions with Compositionally Optimized PdAu Nanoparticle Catalysts in Raspberry Colloid-Templated SiO2},
  year = {2020},
  journal = {ACS Catalysis},
  author = {Luneau, M. and Shirman, T. and Foucher, Alexandre C. and Duanmu, Kaining and Verbart, David M. A. and Sautet, P. and Stach, E. and Aizenberg, J. and Madix, R. and Friend, C.}
}

Abstract

Improving the selectivity for catalytic hydrogenation of alkynes is a key step in upgrading feedstocks for olefin polymerization. Herein, dilute PdxAu1-x alloy nanoparticles embedded in raspberry colloid templated silica (x=0.02, 0.04, and 0.09) are demonstrated to be highly active and selective for the gas-phase hydrogenation of 1-hexyne, exhibiting higher selectivity than pure Pd at high conversion. The conversion of 1-hexyne remains high even for the very low amounts of Pd in Pd0.02Au0.98. These catalysts are highly resistant to sintering—addressing a long-standing challenge in the use of Au-based catalysts. Clear evidence is presented that the addition of the second hydrogen to the half-hydrogenated intermediate is the rate-limiting step, and that the stability of the half-hydrogenated intermediate of the alkyne is higher than the half-hydrogenated alkene which explains the high selectivity even at high conversions. Moreover, of the three compositions investigated, optimum selectivity and activity is ...


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