Achieving enhanced and robust propane selective oxidative dehydrogenation via electrically-driven continuous chemical...

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 CO_x, 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 La_0.6Sr_0.4Co_0.2Fe_0.8O_3-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 g_total^-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 O^2- 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.