초록/요약

Shale-gas-derived methyl acetate (MA) production is an energy-efficient value-added chemical process. Therefore, we first simulated dimethyl ether (DME) production process from shale-gas-derived syngas (CO/H-2) by controlling the syngas composition using a membrane separation process and then converted the resulting DME into MA as a proof-of-concept strategy. Our proposed integrated MA synthesis process consisted of syngas production (including Matrimid (R) 5218 membrane separation), DME production/separation (Cu-ZnO-Al2O3/ferrierite catalyst), and MA production/separation (FER@FER catalyst). In addition, the DME-based MA yield and selectivity were determined using a fixed-bed reactor, and the results were applied to the Aspen Plus (TM) simulator to describe the overall MA production process from shale-gas. Our proposed MA production process enabled continuous MA production from shale gas and simultaneous H-2 production. Furthermore, the proposed catalyst increased MA selectivity to 97% and exhibited relatively high conversion (27.82%) of DME to MA in excess CO. Most importantly, our rigorously mathematically modeled technoeconomic analysis (TEA) estimated that the MA production costs were approximately 0.71, 0.64, 0.60, and 0.63 $/kg MA for dry reforming of methane, partial oxidation, steam reforming of methane, and tri-reforming of methane syngas production methods, respectively. The net present values (NPVs) of the respective processes were 617, 525, 667, and 835 MM$ during 30 years of plant operation. Such low MA production costs and relatively high NPVs were comparable to those of the most mature conventional MA production processes (0.95 $/kg MA) owing to enhanced membrane-separation-based DME production and selective recycling streams, thereby supporting the feasibility of industrially producing MA using syngas-derived DME intermediates.