Super-dry reforming of methane using a tandem electro-thermocatalytic system
摘要
Dry reforming of methane is a well-studied reaction for syngas production from CO2 and CH4. While the reaction is normally performed at a feed ratio of one, the envisioned future feedstocks contain far more CO2 and thus require extensive separation to use the desired CH4. Here we develop a three-step tandem electro-thermocatalytic CH4 reforming reaction for converting CO2-rich natural gas. The combination of the tandem CH4 reforming process with the reverse water–gas shift reaction and an oxygen-ion-conducting electrolysis-membrane reactor, in which water electrolysis shifts the equilibrium of the reverse water–gas shift reaction, promotes syngas production and increases the apparent CH4 reducibility. The catalyst, formed from the in situ exsolution of Rh nanoparticles on a CeO2–x support, provides substantial Ce3+–VO–Rhδ+ interfacial active sites for high catalytic performances. This tandem system used up to four CO2 molecules per CH4 molecule, afforded high CH4 and CO2 conversions and yielded high selectivity for CO and H2 production.