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Super-dry reforming of methane intensifies CO2 utilization via Le Chatelier’s principle

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Science  13 Oct 2016:
aah7161
DOI: 10.1126/science.aah7161

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Abstract

Efficient CO2 transformation from a waste product to carbon source for chemicals and fuels will require reaction conditions that effect its reduction. We develop a “super-dry” CH4 reforming reaction for enhanced CO production from CH4 and CO2. We used Ni/MgAl2O4 as a CH4 reforming catalyst, Fe2O3/MgAl2O4 as a solid oxygen carrier, and CaO/Al2O3 as a CO2 sorbent. The isothermal coupling of these three different processes resulted in higher CO production compared with conventional dry reforming by avoiding back reactions with water. The reduction of iron oxide was intensified by CH4 conversion to syngas over Ni and by CO2 extraction and storage as CaCO3. CO2 is then used for iron reoxidation and CO production exploiting equilibrium shifts effected with inert gas sweeping (Le Chatelier’s Principle). Super-dry reforming utilizes up to three CO2 molecules per CH4 and offers a high CO space-time yield of 7.5 mmol CO per second per kilogram of iron at at 1023 Kelvin.

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