Evaluation of multi-cycle performance of chemical looping dry reforming using CO_2 as an oxidant with Fe–Ni bimetallic oxides

Chemical looping dry reforming（CLDR） is an innovative technology for CO2 utilization using the chemical looping principle.The CLDR process consists of three stages,i.e.CH4 reduction,CO2 reforming,and air oxidation.Spinel nickel ferrite（NiFe2O4） was prepared and its multi-cycle performance as an oxygen carrier for CLDR was experimentally investigated.X-ray diffraction（XRD） and Laser Raman spectroscopy showed that a pure spinel crystalline phase（NiFe2O4） was obtained by a parallel flow co-precipitating method.NiFe2O4was reduced into Fe-Ni alloy and wustite（FexO） during the CH4 reduction process.Subsequent oxidation of the reduced oxygen carrier was performed with CO2 as an oxidant to form an intermediate state：a mixture of spinel Ni（1-x）Fe（2＋x）O4,Fe（2＋y）O4 and metallic Ni.And CO was generated in parallel during this stage.Approximate 185 mL of CO was generated for 1 g spinel NiFe2O4 in a single cycle.The intermediate oxygen carrier was fully oxidized in the air oxidation stage to form a mixture of Ni（1＋x）Fe（2-x）O4 and Fe2O3.Although the original state of oxygen carrier（NiFe2O4） was not fully regenerated and agglomeration was observed,a good recyclability was shown in 10 successive redox cycles.