Gas-Phase Catalytic Hydrogenation/Isomerization in the Transformation of 3-Butyn-2-ol over Pd-Ni/Al2O3

Alberto González-Fernández, Chiara Pischetola, Fernando Cardenas-Lizana

Research output: Contribution to journalArticlepeer-review

Abstract

The continuous gas-phase (P = 1 atm; T = 373 K) hydrogenation of 3-butyn-2-ol has been investigated over Pd/Al2O3 and Ni/Al2O3 prepared by incipient wetness impregnation and Pd–Ni/Al2O3 (Pd/Ni mol ratio = 1:1) synthesized by co-impregnation. A physical mixture (Pd/Al2O3 + Ni/Al2O3; Pd/Ni = 1:1) is also considered for comparison purposes. H2 temperature-programmed reduction (TPR) results are consistent with a lower temperature requirement for the reduction of palladium and nickel in the bimetallic catalyst relative to the monometallic counterparts. The Pd/Al2O3 catalyst exhibits a narrow metal particle size distribution (mean = 20 nm) while Ni/Al2O3 and Pd–Ni/Al2O3 bore larger particles (mean = 28 ± 2 nm). TEM–EDX, XRD, and XPS measurements are consistent with a palladium surface-enriched Pd–Ni bimetallic phase. Ni/Al2O3 promoted exclusive −C≡C– group hydrogenation to generate 3-buten-2-ol (partial reduction) and 2-butanol (complete reduction). Pd/Al2O3 exhibited a greater H2 uptake and delivered a higher 3-butyn-2-ol transformation rate, yielding 3-buten-2-ol, 2-butanol, and 2-butanone through hydrogenation and double bond migration. An equivalent H2 uptake, rate, and product distribution were delivered by Pd/Al2O3 and the Pd/Al2O3 + Ni/Al2O3 system, where the catalytic response was controlled by the palladium component. In contrast, we recorded a higher hydrogen chemisorption on Pd–Ni/Al2O3 (vs Pd/Al2O3) and catalytic activity with an enhanced selectivity to 3-buten-2-ol (up to 95%). We linked the distinct response over Pd–Ni/Al2O3 to the formation of bimetallic Pd–Ni as proven by TPR, XRD, TEM–EDX, and XPS analyses. A parallel/stepwise kinetic model has been used to quantify the catalytic hydrogenation response.
Original languageEnglish
Pages (from-to)2454-2463
Number of pages10
JournalJournal of Physical Chemistry C
Volume125
Issue number4
Early online date26 Jan 2021
DOIs
Publication statusPublished - 4 Feb 2021

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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