Search

The integrated synergistic effect of the ligand and the strong metal-support interaction (SMSI) effectively improves the selectivity and stability of heterogeneous Pd-based catalysts for acetylene dicarbonylation under high-pressure CO conditions. [Display omitted] • Stabilizing the catalytic active site Pdδ+ for acetylene dialkoxycarbonylation. • Oxygen-containing functional groups of AC provide anchoring sites for stabilize active Pd2+ ions. • The coordination of I- not only accelerates the reaction but also stabilizes the catalyst. The support and ligand play a crucial role in regulating the catalytic performance, selectivity, and stability of heterogeneous catalysis. Herein, activated carbon (AC) supported palladium (Pd) catalysts (2.0 wt%) were prepared by impregnation for acetylene dicarbonylation. The oxygen-containing groups on the surface of the AC support were modulated by nitric acid (HNO 3) to investigate metal–support interactions on the catalytic performance and stability of the Pd/AC. The characterization of the chemical composition and structure of the supports and catalysts demonstrates that high concentrations of oxygen-containing groups on the surface of the carbon support lead to the fine dispersion of Pd nanoparticles. Notably, the finely dispersed Pd/AC 70 catalyst exhibited good activity and stability for acetylene dicarbonylation under high-pressure CO conditions after several rounds of regeneration. Furthermore, operational parameters including the type of support, co-catalyst (KI), and reaction time and temperature were identified for their impact on the reaction. It was found that I- anions serve as a co-catalyst and can ligate with Pd species, thereby preventing the leaching of Pd and improving reaction selectivity. This study presents a straightforward and sustainable modulation strategy to improve the dispersion of active metals, as well as to prevent the leaching and sintering of these metals during high-pressure CO reactions. [ABSTRACT FROM AUTHOR]