Pd-CuxO Synergetic Catalysis towards High-Efficient Oxidative Carbonylation of Ethanol

Oxidative carbonylation of ethanol to diethyl carbonate (DEC), an essential electrolyte for lithium-ion battery, has attracted broad interest from both academia and industry in recent years. But high selective formation of DEC is a great challenge due to the difficulty in efficient activation of CO at the same time as the site-specific activation of O—H bond in ethanol. Herein, we propose a Pd-Cu x O synergetic catalysis toward oxidative carbonylation of ethanol, where the synergy between Pd and Cu x O promotes CO activation and carbonylation, thus increasing the selectivity to the site-specific activation of O-H bond in ethanol. A nitrogen-doped carbon nanotubes supported Pd-Cu x O (Pd-Cu x O/NCNTs) has been designed via galvanic displacement of Pd on Cu x O to form the strong interactions between Pd and Cu x O, affording a selectivity of 94.7 % to DEC and a space-time yield (STY) of up to 5966 mg∙g –1 ∙h –1 , which is an order of magnitude higher than that reported in the literatures. This work offers novel insights for the design of highly efficient catalysts and advances the industrial development for the oxidative carbonylation of ethanol.