Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts

Emmett Goodman, Allegra A. Latimer, An-Chih Yang, Liheng Wu, Nadia Tahsini, Frank Abild-Pedersen, Matteo Cargnello
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ACS Applied Nano Materials

The low-temperature conversion of methane into value-added products is an appealing goal due to the abundance of methane in the form of natural gas. Industrially, methane is used to produce synthesis gas (syngas), a precursor mixture used heavily in the production of ammonia, methanol, and synthetic fuels. In practice, this mixture is produced via the energy-intensive methane steam reforming reaction at temperatures between 750 and 1450 °C. The exothermic methane partial oxidation reaction stands as an alternative for syngas formation at lower temperatures, especially for gas to liquid fuels applications, yet awaits large-scale implementation due to dangerous operating conditions and temperatures. Using colloidally synthesized Ru catalysts, we identify two unifying rules that govern the low-temperature production of synthesis gas: depletion of oxygen within the catalyst bed and facile RuO2 → Ru reduction kinetics, which is a strong function of supporting material and Ru nanostructure. Using these design rules, we demonstrate the enhanced low-temperature activity of a bifunctional Ru/Pd catalyst which produces synthesis gas at ∼400 °C, with nearly complete CH4 conversion and CO selectivity at 670 °C.

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