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Carbon‐supported Au catalyst in Acetylene Hydrochlorination: Enhancing Catalytic Performance by Complexation of Dicarbonyl Ligands

Von Wiley-VCH zur Verfügung gestellt

Carbon-supported Au (Au/AC) catalyst has been proven to be one of the most promising catalysts in the field of acetylene hydrochlorination. However, the catalytic performance of conventional Au/AC catalyst is usually limited due to the unsatisfactory dispersion of active Au cation on the surface of the support, carbon deposition, and inevitable reduction to inactive Au nanoparticles. Herein, Au catalysts with highly dispersed Au cation were developed using the complexation of dicarbonyl ligand N-Chlorosuccinimide (NCS) and N-Methylsuccinimide (NMS). The obtained Au-NMS/AC and Au-NCS/AC catalysts with 0.1 wt. % Au loading possessed acetylene conversion of 98% and 88% at 180 °C and GHSV (C2H2) of 160 h‒1, which were clearly better than that of pristine Au/AC. The characterization results showed that coordination between Au cation and ligands enhanced the dispersion of Au species, suppressed the reduction of Au cation, and reduced the formation of carbon deposits. Density functional theory (DFT) calculations suggested that Au-NMS/AC and Au-NCS/AC catalysts follow a HCl-preferred concerted addition reaction mechanism with lower reaction energy barrier. This favors the high activity and nuclearity stability of the Au center. This study provided great potential for the use of dicarbonyl ligands on Au-based catalysts in acetylene hydrochlorination.

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