Publication date: 10th April 2024
Chemical looping for hydrogen production (CLHP) shows the potential to substantially lower the CO2 emissions from H2 production with hydrocarbon sources [1]. In CLHP, an oxygen-carrying material (OCM) is reduced by a hydrocarbon source to produce syngas, followed by partly oxidation with steam to generate pure H2, before re-oxidation with air to balance the energy demand [2]. However, commercialization of CLHP is still limited by the OCM which should possess a demanding set of properties; catalytic activity towards the red-ox processes without forming coke, sufficient oxygen transport and storage capacity, chemical and microstructural stability over numerous redox cycles, and be abundant with no environmental and societal issues [3].
Ca/Sr1-xLaxBO3 (B = Ti, Cr, Mn, Co, or Fe) perovskites are interesting OCM candidates, showing good chemical stability, high mixed ionic- and electronic conductivity and reversible oxygen stoichiometry over a wide range of reaction conditions[4-6]. In this work, a matrix of Ca0.6La0.4Ti0.1CrxMn0.9-xO3-δ, x = 0, 0.3, 0.45 and 0.9, has been studied to investigate the effects of the Cr/Mn content on oxygen exchange kinetic, chemical stability and oxygen stoichiometry.
Pulse Isotope Exchange measurement was utilized to investigate the oxygen exchange of the different compositions as a function of pO2 and temperatures to determine the total oxygen exchange rate (ℜ0), as well as, rates for dissociative adsorption (ℜa) and incorporation (ℜi). Chemical stability and oxygen stoichiometry of the different compositions were tested by thermogravimetric analysis under simulated CLHP operating conditions, followed by XRD and SEM.
These novel materials show excellent chemical stability and adequate regenerative oxygen stoichiometry over the whole CLHP range, of which Ca0.6La0.4Ti0.1Cr0.3Mn0.6O3-δ exhibits the best overall performance. Variations in the oxygen exchange kinetics and capacity, and the chemical stability, will be discussed with basis in the material’s point defect thermodynamics.
This study was performed as part of the OxHyPro project "Novel oxygen carriers in sustainable hydrogen production ", under the CLIMIT programme; the grant application no. 315083 funded by the Research Council of Norway.
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