Achieving enhanced and robust propane selective oxidative dehydrogenation via electrically-driven continuous chemical looping
摘要
Oxidative propane dehydrogenation (OPDH) has emerged as a promising approach for direct propylene production. However, it still confronts great challenge of overoxidation of propane to COx, damaging the products selectivity. Herein, we report an electrically-driven continuous chemical looping process to efficiently produce propylene via an electrochemical CO2-OPDH system within solid oxide electrolysis cells (SOECs). At an optimal current density of 10 mA cm−2, the system with a Co3O4-modified La0.6Sr0.4Co0.2Fe0.8O3-δ (LSCF) anode achieves 92.6% olefin selectivity and 14.2% single-pass propane conversion. This current-driven configuration boosts the propylene yield (5.11 mmol gtotal−1 h−1) by a factor of 18.5 over the open-circuit baseline. The electrochemical CO2-ODHP system also exhibits good stability during a 120-hour durability test. In-situ characterization and theoretical calculations elucidate the electrically driven online replenishment mechanism of Co3O4 lattice oxygen by O2- derived from cathode CO2 reduction. This dynamic cycle maintains moderate anode surface oxygen activity, resulting in highly efficient and selective OPDH without significant over-oxidation or cracking of propane.