Co-doping of Li/MgO, a well-known catalyst for the oxidative coupling of methane, was investigated. It is demonstrated that Gd3+ and Fe3+ can be used as spin sensors in these solids to investigate the structure via EPR spectroscopy. These aliovalent ions occupy Mg2+ sites in the lattice; the expected coupling with charge-compensating neighboring Li+ was detected. A strong increase of the activity was observed. However, all samples suffered from deactivation. The solubility of Gd3+ in MgO turned out to be inhibited. No such restriction was observed for Fe3+.
