Three-dimensionally ordered macroporous La0.6Sr0.4MnO3 with high surface areas: Active catalysts for the combustion of methane

• Published in: Journal of catalysis Vol. 307; pp. 327 - 339
• Main Authors: Arandiyan, Hamidreza, Dai, Hongxing, Deng, Jiguang, Liu, Yuxi, Bai, Bingyang, Wang, Yuan, Li, Xinwei, Xie, Shaohua, Li, Junhua
• Format: Journal Article
• Language: English
• Published: Amsterdam Elsevier Inc 01.11.2013; Elsevier; Elsevier BV
• Subjects: activation energy; analytical methods; Catalysis; Catalysts; catalytic activity; Chemical synthesis; Chemistry; Colloidal state and disperse state; combustion; composite polymers; ethylene glycol; Exact sciences and technology; General and physical chemistry; glycols; Low-temperature reducibility; lysine; Methane; Methane combustion; oxygen; physicochemical properties; polyethylene glycol; Polymethyl methacrylate-templating preparation; polymethylmethacrylate; Porous materials; surface area; Surfactant-mediated fabrication; surfactants; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry; Three-dimensionally ordered macroporous La0.6Sr0.4MnO3; Low-temperature reducibility; Polymethyl methacrylate-templating preparation; Surfactant-mediated fabrication; Methane combustion; Three-dimensionally ordered macroporous La0.6Sr0.4MnO3; Methane; Reducibility; Lanthanum Oxides; Methyl methacrylate polymer; Combustion; Surfactant; Porous material; Three-dimensionally ordered macroporous; Template; La; Low temperature; Transition element compounds; MnO; Heterogeneous catalysis; Quaternary compound; Preparation; Manganese Oxides; Surface area; Strontium Oxides; Catalyst; Macroporosity; Sr
• ISSN: 0021-9517; 1090-2694
• DOI: 10.1016/j.jcat.2013.07.013

Rhombohedrally crystallized3DOM La0.6Sr0.4MnO3 (LSMO) catalysts with a high surface area of 32–42m2/g were prepared by the PMMA-templating method. The 3DOM LSMO-DP3 catalyst derived with 3.0mL of dimethoxytetraethylene glycol and 5.0mL of polyethylene glycol shows excellent activity for the combustion of methane. [Display omitted] •High-surface-area 3DOM La0.6Sr0.4MnO3 is prepared by the PMMA-templating method.•Surfactant addition is critical in 3DOM structure formation with nanovoid-like walls.•The calcination procedure is a key step in the formation of 3DOM structure.•3DOM La0.6Sr0.4MnO3-DP3 performs best in the combustion of methane.•Surface area, Oads, and reducibility determine the activity of 3DOM La0.6Sr0.4MnO3. Three-dimensionally ordered macroporous rhombohedral La0.6Sr0.4MnO3 (3DOM LSMO) with nanovoids was prepared using polymethyl methacrylate (PMMA) microspheres as a hard template and dimethoxytetraethylene glycol (DMOTEG), ethylene glycol, polyethylene glycol (PEG400), l-lysine, or triblock copolymer (Pluronic P123) as a surfactant. Physicochemical properties of the materials were characterized by a number of analytical techniques, and their catalytic activities for the combustion of methane were evaluated. It is shown that the morphology of the sample depended strongly on the nature of the surfactant added during the fabrication process. The macropore sizes and surface areas of the 3DOM LSMO materials were 165–214nm and 32–40m2/g, respectively. It is found that addition of appropriate amounts of DMOTEG and PEG400 was beneficial for the generation of high-quality 3DOM-structured La0.6Sr0.4MnO3 (denoted as LSMO-DP1, LSMO-DP3, LSMO-DP5, derived with a DMOTEG /PEG400 ratio of 0.2, 0.6, and 1.0, respectively). The LSMO-DP3 catalyst derived with 3.0mL of DMOTEG and 5.0mL of PEG400 possessed the highest oxygen species concentration and surface area and best low-temperature reducibility, and hence exhibited a good catalytic activity (T10%=437°C, T50%=566°C, andT90%=661°C at GHSV=30,000mL/(gh)) for methane combustion. The apparent activation energies of the 3DOM LSMO samples were estimated to be 56.5–75.2kJ/mol, with the LSMO-DP3 sample showing the lowest apparent activation energy (56.6kJ/mol).