A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Ligand assisted hydrogenation of levulinic acid on Pt(111) from first principles calculations (2022)

Gell, L., & Honkala, K. (2022). Ligand assisted hydrogenation of levulinic acid on Pt(111) from first principles calculations. Catalysis Science and Technology, 12(6), 1850-1858. https://doi.org/10.1039/D1CY02048J

JYU-tekijät tai -toimittajat

Gell, Lars
Honkala, Karoliina

Julkaisun tiedot

Julkaisun kaikki tekijät tai toimittajat: Gell, Lars; Honkala, Karoliina

Lehti tai sarja: Catalysis Science and Technology

ISSN: 2044-4753

eISSN: 2044-4761

Julkaisuvuosi: 2022

Volyymi: 12

Lehden numero: 6

Artikkelin sivunumerot: 1850-1858

Kustantaja: Royal Society of Chemistry

Julkaisumaa: Britannia

Julkaisun kieli: englanti

DOI: https://doi.org/10.1039/D1CY02048J

Julkaisun avoin saatavuus: Avoimesti saatavilla

Julkaisukanavan avoin saatavuus: Osittain avoin julkaisukanava

Julkaisu on rinnakkaistallennettu (JYX): https://jyx.jyu.fi/handle/123456789/80163

Tiivistelmä

In this study, we investigate the hydrogenation reaction of levulinic acid to 4-hydroxypentanoic acid on ligand-modified Pt(111) using DFT. Modifying nanoparticle surfaces with ligands can have beneficial effects on the desired reaction such as improved selectivity or lower activation energies. The N3,N3-dimethyl-N2-(quinolin-2-yl)propane-1,2-diamine (AQ) ligand was selected to modify the surface, since it combines good surface adsorption properties with functional groups that can influence the reaction. The adsorption geometry of the AQ ligand was studied as well as the co-adsorption of a second AQ ligand for the possibility of self-assembly. We found that dissociated hydrogen from the Pt(111) surface can protonate the AQ ligand and discuss the role this plays on the mechanism of the hydrogenation reaction of levulinic acid (LA). By comparing the ligand-modified Pt(111) surface to the bare Pt(111) surface we show that the reaction changes from a step-wise to a concerted mechanism due to the influence of the ligand molecule. This demonstrates the effect that ligand-modified surfaces can have on catalyzing reactions and shows that desired reactions can be achieved by tuning the reaction environment.

YSO-asiasanat: hydraus; katalyysi; katalyytit; nanohiukkaset; platina