Oxidative coupling of biogas to ethylene over a trilobe-shaped Mn-Na2WO4/α-Al2O3 catalyst in a single-pellet reactor

Abstract

Despite the development of selective catalyst formulations for oxidative coupling of methane (OCM), kinetic and reactor design studies have been hampered by a lack of data for truly isothermal reaction conditions. Because of the high exothermicity, the temperature of a fixed-bed reactor filled with Mn-Na2WO4/SiO2 catalysts will show hot-spots with a loss of selectivity. The objective of this study is to measure catalyst activity under relevant reaction conditions of pressure (3 bar), biogas composition (no dilution) and contact time, while keeping the process isothermal. To this aim, we have synthesized and shaped a trilobed Mn-Na2WO4/α-Al2O3 catalyst, which may be used as is at industrial scale, and measured its performance in a single-pellet reactor. We found that the presence of CO2 did not degrade the catalyst performance, even on the long run, which should enable the use of a CO2-rich stream such as biogas. Actually, higher methane conversions have been obtained in the presence of CO2, likely due to a possible contribution of methane dry reforming reaction. We also noticed a slow catalyst activation over the first 100 h, while selectivity was kept constant.