Improvement of Process Conditions for H₂ Production by Chemical Looping Reforming

A syngas production process was studied cyclically, exploiting the redox properties of Ce-based oxygen carriers. The two steps of the looping cycle were investigated through thermogravimetric analysis and fixed bed experiments. While TGA experiments were focused on the identification of the optimal temperatures ranges for methane partial oxidation (900–1000 °C) and carrier regeneration (400–900 °C), fixed bed testing was performed isothermally (at 900 or 950 °C), with a 10% CH4 feed stream in N2 to investigate material stability and cyclic performance reproducibility. The effect of the process times on carbon deposition, specific syngas yields, and selectivity was inspected, together with the investigation of best conditions to fully regenerate the carrier, adjust the syngas final ratio, and to ensure stable performances. The obtained results ensured the possibility to work in fully isothermal operations, with CH4 conversion of up to 38% and specific yields of syngas per mass of O2 carrier between 4.0–6.8 mmol∙g−1, preserved even across cycles, thus paving the path to the development of alternative and effective processes for syngas production. Under the operating conditions of the lab-scale experiment, an effective reforming time was 20 min, corresponding to 1.16 times of the characteristic time of reaction kinetics at 950 °C.