Control of the single atom/nanoparticle ratio in Pd/C catalysts to optimize the cooperative hydrogenation of alkenes - Archive ouverte HAL Access content directly
Journal Articles Catalysis Science & Technology Year : 2021

Control of the single atom/nanoparticle ratio in Pd/C catalysts to optimize the cooperative hydrogenation of alkenes

R. Philippe
Philippe Serp

Abstract

We recently reported (R. Castro Contreras, B. Guicheret, B. F. Machado, C. Rivera-Cárcamo, M. A. Curiel Alvarez, B. Valdez Salas, M. Ruttert, T. Placke, A. Favre Réguillon, L. Vanoye, C. de Bellefon, R. Philippe and P. Serp, J. Catal., 2019, 372, 226–244) that a structure/activity correlation exists in Pd/C catalysts for myrcene hydrogenation, which integrates the Pd dispersion, and the surface concentration of oxygen groups and defects of the support. Here, through a combined experimental–theoretical study, we provide an explanation of the influence of these three structural characteristics of Pd/C catalysts for alkene hydrogenation. Highly dispersed Pd nanoparticles (PdNP) are necessary to activate dihydrogen. A high concentration of surface defects on the support is necessary to stabilize Pd single atoms (PdSA), which coexist with PdNP on Pd/C catalysts. A high concentration of oxygenated surface groups is also necessary on the support to allow hydrogen spillover. We demonstrate that such a combination allows cooperative catalysis to operate between PdNP and PdSA that involves the formation of PdSA–H species, which are much more active than PdNP–H for alkene hydrogenation but also isomerization. Importantly, we also report an efficient method to control the ratio between PdSA and PdNP in Pd/C catalysts of similar loadings and show that the control of this ratio allows the development of a new generation of stable and highly active catalysts integrating the ultra-rational use of precious metals in short supply. Indeed, for myrcene hydrogenation, activity variations of several orders of magnitude were measured as a function of the value of this ratio.
Fichier principal
Vignette du fichier
Proof_Catal_Sci_Technol.pdf (3.23 Mo) Télécharger le fichier
Origin : Files produced by the author(s)

Dates and versions

hal-03148510 , version 1 (10-11-2021)

Identifiers

Cite

Camila Rivera‐cárcamo, I.C. Gerber, Iker Del rosal, B. Guicheret, Rubén Castro Contreras, et al.. Control of the single atom/nanoparticle ratio in Pd/C catalysts to optimize the cooperative hydrogenation of alkenes. Catalysis Science & Technology, 2021, 11 (3), pp.984-999. ⟨10.1039/d0cy01938k⟩. ⟨hal-03148510⟩
78 View
132 Download

Altmetric

Share

Gmail Facebook Twitter LinkedIn More