Kinetics of liquid-phase diphenylacetylene hydrogenation on “single-atom alloy” Pd-Ag catalyst: Experimental study and kinetic analysis

Alexander V. Rassolov, Igor S. Mashkovsky, Galina O. Bragina, Galina N. Baeva, Pavel V. Markov, Nadezhda S. Smirnova, Johan Wärnå, Alexander Yu Stakheev, Dmitry Yu Murzin*

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

Abstract

Catalytic performance of Pd1Ag3/Al2O3 single-atom alloy (SAA) catalyst was studied in liquid-phase hydrogenation of diphenylacetylene (DPA) and compared with the performance of the reference monometallic Pd/Al2O3. Formation of SAA structure in Pd1Ag3/Al2O3 was confirmed by FTIR CO technique. It was found that Pd1Ag3/Al2O3 single-atom alloy catalyst exhibits excellent selectivity in diphenylethene (stilbene) (ca. 98 %), which remains constant over a wide range of DPA conversions (0–95%), while over Pd/Al2O3 selectivity decreases steadily with the increase in DPA conversion. It is remarkable that the selectivity of Pd1Ag3/Al2O3 depends neither on hydrogen pressure (5–15 bar), nor on DPA concentration (0.0262 – 0.159 mol/l). In contrast, over the reference Pd/Al2O3 selectivity tends to decrease with increasing P(H2) and decreasing DPA concentration. The proposed reaction network comprises hydrogenation of DPA in a parallel formation of cis and trans-stilbene with following hydrogenation to bibenzyl and direct formation of the latter from the initial DPA. The calculations clearly shows the capability of the kinetic model to describe the experimental dependencies for Pd1Ag3 single-atom catalyst in an excellent way with the degree of explanation equal to ca. 99 %.

Original languageEnglish
Article number111550
JournalMolecular Catalysis
Volume506
DOIs
Publication statusPublished - Apr 2021
MoE publication typeA1 Journal article-refereed

Keywords

  • Diphenylacetylene
  • Hydrogenation
  • Kinetics
  • Selectivity
  • Single-atom catalysis

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