<p>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<sub>x</sub>/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. <i>Operando</i> X-ray absorption spectroscopy and in situ spectroscopies reveal the progressive reduction of NiO to metallic Ni and its controlled carburization into Ni<sub>x</sub>C, 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.</p>

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

  • Xuan Gong,
  • Xinhuilan Wang,
  • Alejandra Rendón-Patiño,
  • Natalia Morlanes,
  • Ahmed Alamer,
  • Abdallah Nassereddine,
  • Antonio Aguilar Tapia,
  • Edy Abou-Hamad,
  • Selvedin Telalović,
  • Khairova Rushana,
  • Orxan Sayidov,
  • Jean-Louis Hazemann,
  • Mohnnad H. Alabsi,
  • Jean Marcel R. Gallo,
  • Jorge Gascon

摘要

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 NiOx/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 NixC, 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.