Enhanced catalytic performance in acetylene hydration: A novel Cu-based catalyst anchored via P-O bonds on a CN supporter

Abstract

Despite various catalysts being developed for acetylene hydration, challenges persist in achieving optimal selectivity and stability. In this report, we present a catalyst featuring the active component Cu-O3P3 attached to a nitrogen-dispersed carbon carrier (Cu-O3P3/CN) by self-assembly. Over this catalyst, the acetaldehyde selectivity of 88.2 % for acetylene hydration could still be obtained at 126 h (T = 240°C, GHSV(C2H2) = 90 h-1 and VH2O/VC2H2 = 4). Transmission Electron Microscopy, X-ray Photoelectron Spectroscopy, and X-ray Diffraction analyze that the employed preparation method thoroughly prevents the reduction of high-valent Cu during the fabrication process. The construction of the specific Cu-O3P3 active site structure has been demonstrated by X-ray absorption fine structure and X-ray photoelectron spectroscopy tests. Density functional theory calculations confirm active Cu sites are modified to a more electron-deficient state by constructing Cu-O-P sites. Furthermore, the doping of the carbon carrier with heteroatom nitrogen may theoretically lead to a reduction in the energy barrier associated with the formation of intermediates and the desorption of products, thereby potentially enhancing the overall catalytic performance. This study introduces a versatile methodology for designing and developing well-defined, carbon-nitrogen-supported Cu-based catalysts and a strategy for fine-tuning their catalytic characteristics.