Spatiotemporal activation of Ni/Zeolite catalysts enables isoparaffin-rich gasoline

The direct conversion of dimethyl ether (DME) to liquid fuels offers an attractive single-step route to high-octane gasoline. However, achieving the required synergy between metal and acid functions remains a long-standing challenge: Ni promotes hydrogenation but also triggers unselective hydrogenolysis, while zeolite acid sites initiate C-C coupling yet suffer from rapid deactivation. Here we report an induction-programming strategy that dynamically transforms NiO_x/ZSM-5 into a cooperative Ni/NiₓC/zeolite interface under reaction conditions. This interface suppresses methane and aromatics formation, while directing the reaction pathway toward branched isoparaffins with high yield and stability. Operando X-ray absorption spectroscopy and in situ spectroscopies reveal the progressive reduction of NiO to metallic Ni and its controlled carburization into Ni_xC, correlating phase evolution with the onset of selective tandem catalysis. Through control of the active phase's temporal evolution, induction programming offers a versatile framework for activating bifunctional catalysts and achieving spatiotemporal control of complex reactions beyond DME conversion.