LAUSR

In industrial zeolite catalysis, high‐temperature (>650°C) air combustion is commonly used to restore the activity of catalysts deactivated by coke deposition. Herein, we propose a low‐temperature (440–500°C) air regeneration strategy that harnesses spatially restructured coke in SAPO‐34 catalysts for enhanced performance in the methanol‐to‐olefins reaction. The resulting “tight‐outside, loose‐inside” coke distribution expands accessible reaction volumes, improves product transport, and enhances exposure of confined naphthalene species, key intermediates for ethylene formation. Compared to conventional high‐temperature air regeneration that substantially removes coke, the proposed strategy repurposes it as a functional promoter, enabling prolonged catalyst lifetime and markedly improved ethylene selectivity. The practical viability of this strategy was further confirmed by pilot‐scale fluidized bed reactor‐regenerator experiments and process simulations in terms of both catalyst stability and thermal utilization efficiency. This work reveals an alternative approach to enhance shape‐selective zeolite catalysis via rationally modulating coke by controlling the regeneration strategy.