More Efficient Ethanol Synthesis from Dimethyl Ether and Syngas over the Combined Nano-Sized ZSM-35 Zeolite with CuZnAl Catalyst

Converting syngas into ethanol (EtOH) is highly attractive but remains challenge. Dimethyl ether (DME) carbonylation with CO to methyl acetate (MA) on zeolite and its further hydrogenation to EtOH on Cu-based catalyst open a new EtOH synthesis route from syngas. In this work, a nano-sized ZSM-35 (NZ35) zeolite, possessing abundant active sites and porosity and short diffusion path, is found to realize much better activity of DME to MA than that of the conventional ZSM-35 zeolite (CZ35). In addition, a simple formic-acid-assisted solidstate method is employed for preparation an auto-reduced CuZnAl (CZAargon) catalyst under argon atmosphere. The prepared CZAargon catalyst exhibits an excellent catalytic activity for conversion of produced MA to EtOH. By investigating the effects of different integration manners of NZ35 zeolite and CZAargon catalyst, we find that EtOH can be synthesized only when the NZ35 zeolite and CZAargon catalyst pack in a dual-catalyst bed reactor. After optimizing the reaction conditions for EtOH synthesis with the combination of NZ35 zeolite and CZAargon catalyst, it is found that the DME conversion and MA selectivity are stabilized at 47.0 % and 45.6 % respectively, at 220 C and 2.5 MPa.