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.

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

http://science.sciencemag.org/content/early/2016/10/12/science.aah7161.full