(583be) Catalytic Oxidative Carbonylation Over Cu Nanoclusters Supported On Carbon Materials: Effect of Carbon Support

Yan, B. - Presenter, Massachusetts Institute of Technology
Wang, S., Tianjin University
Ma, X., Tianjin University
Gong, J., Tianjin University
Wang, J., Tianjin University

Carbon supported Cu-based catalysts have exhibited excellent catalytic performance in dialkyl carbonates, especially for dimethyl carbonate (DMC) and diethyl carbonate (DEC) synthesis by catalytic oxidative carbonylation. In this talk, we will discuss about the effect of structure and the role of surface oxygen containing groups (OCGs) of carbon support. With investigation over ordered mesopores carbons (OMCs) and activated carbon (AC) supporting CuCl2/PdCl2 catalysts, we have obtained the effect of support structure on catalyst catalytic performance. TEM, SEM, as well as XRD results have indicated that ordered mesopore structure of OMCs are favorable for dispersion of the active components. And the ethanol conversion of the catalysts was improved by ~65% using OMCs as the catalyst support than AC. We have also studied the role of OCGs in this catalytic system. Obvious differences of catalytic properties of CuOx supported on zeolite (MCM-41) and carbon materials (granphene and AC) have indicated that OCGs play a key role in catalytic reaction. Catalytic activity data has shown that the active specie in the reaction was the one that OCGs coordinated with CuOx species, which we can call a work cell. The content of OCGs was modulated by treating AC with HNO3, and species of OCGs were controlled by using purified carbon nanotubes (MWNTs-OH and MWNTs-COOH). Qualitative and quantitative relationship between OCGs and catalytic property was established.