Abstract

Dry reforming of methane usually affords low-quality syngas with equimolar amounts of CO and H. Here we report the high conversion of CH and CO to syngas and solid carbon through simultaneous pyrolysis and dry reforming of methane in a bubble column reactor using a molten metal alloy catalyst (65:35 mol% Ni:In). The H to CO ratio can be increased above 1:1 using feed ratios of CH:CO greater than 1:1 to produce stoichiometric solid carbon as a co-product that is separable from the molten metal. A coupled reduction–oxidation cycle is carried out in which CO is reduced by a liquid metal species (for example, In) and methane is partially oxidized to syngas by the metal oxide intermediate (for example, InO), regenerating the native metal. Moreover, the H:CO product ratio can be easily controlled by adjusting the CH:CO feed ratio, temperature, and residence time in the reactor.

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