High Activity of Cu-Co Composite Catalysts Supported on N-Doped Carbon for Dimethyl Carbonate Synthesis via Methanol Oxidative Carbonylation.

Abstract

Copper-based catalysts suffer from sintering and excessive oxidation during the methanol oxidation carbonylation process to produce dimethyl carbonate (DMC), which leads to their easy deactivation and thus are restricted in industrial applications. In this work, we designed and fabricated a series of nitrogen-doped carbon-supported copper-cobalt nanoparticles (CuxCo-NC). A distinctive volcano-type dependence of catalytic activity on the Cu/Co molar ratio was revealed, and a remarkable DMC space-time yield (STY) of 5.35 g g-1 cat·h-1 was delivered by the optimal composition (Cu/Co = 3). There was a strong metal-support interaction between the Cu-Co nanoparticles and the N-doped carbon matrix, promoting the dispersion of the metal. This study has demonstrated the role of ZIF-derived nitrogen-doped carbon materials in the liquid-phase oxidation and carbonylation of methanol, providing a foundation for subsequent research.