Oxidative coupling of methane using catalyst modified dense perovskite membrane reactors

• Published in: Catalysis today Vol. 142; no. 1; pp. 34 - 41
• Main Authors: Olivier, Louis, Haag, Stéphane, Mirodatos, Claude, van Veen, Andre C.
• Format: Journal Article Conference Proceeding
• Language: English
• Published: Amsterdam Elsevier B.V 15.04.2009; Elsevier
• Subjects: BSCFO perovskite; Catalysis; Chemical Sciences; Chemistry; Colloidal state and disperse state; Dense membrane; Environment and Society; Environmental Sciences; Exact sciences and technology; General and physical chemistry; Lanthanum oxide; Membranes; Productivity; Strontium oxide; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry; Productivity; Strontium oxide; Dense membrane; BSCFO perovskite; Lanthanum oxide; Methane; Modification; Perovskite type compound; Membrane surface; Selectivity; Oxidative coupling; Catalytic conversion; Membrane reactor; Membrane; Disk; Oxygen; Catalytic reaction; Hydrocarbon; Magnesium oxide; Catalytic reactor; Heterogeneous catalysis; Models; Catalyst; Comparative study; Natural gas
• ISSN: 0920-5861; 1873-4308
• DOI: 10.1016/j.cattod.2009.01.009

A comparative study modifying an ionic oxygen conducting membrane reactor for the oxidative coupling of methane to higher hydrocarbons with 3 different catalytic surface modifications is presented. Dense Ba 0.5Sr 0.5Co 0.8Fe 0.2O 3− δ (BSCFO) membrane disks were wash-coated with a Pt/MgO model catalyst as well as with more efficient Sr/La 2O 3 and LaSr/CaO catalysts. The role of the catalyst is underlined by the fact that the LaSr/CaO shows that highest yield between 900 and 1000 °C while yields decline for the Sr/La 2O 3 catalyst at temperatures above 900 °C. The latter observation agrees well with observations on conventional catalytic reactors using hydrocarbon/oxygen co-feeding at lower temperature and seems to relate to the formation of highly reactive oxygen species formed at the La 2O 3 surface. Operating a LaSr/CaO modified membrane reactor at 950 °C with a CH 4 concentration of 34%, a C 2-hydrocarbon yield of more than 18% was achieved (at a selectivity of more than 65%). Given the interesting performance, it is obvious that future membrane reactors should employ efficient catalyst systems and development should focus on maximizing the exposure of catalytically modified membrane surfaces.