Highly Active Transition Metal-Promoted CuCeMgAlO Mixed Oxide Catalysts Obtained from Multicationic LDH Precursors for the Total Oxidation of Methane

被引:10
作者
Al-Aani, Hussein Mahdi S. [1 ]
Trandafir, Mihaela M. [2 ]
Fechete, Ioana [3 ]
Leonat, Lucia N. [2 ]
Badea, Mihaela [4 ]
Negrila, Catalin [2 ]
Popescu, Ionel [5 ]
Florea, Mihaela [2 ]
Marcu, Ioan-Cezar [1 ,5 ]
机构
[1] Univ Bucharest, Fac Chem, Dept Organ Chem Biochem & Catalysis, Lab Chem Technol & Catalysis, 4-12 Blv Regina Elisabeta, Bucharest 030018, Romania
[2] Natl Inst Mat Phys, 405A Atomistilor St, Magurele 077125, Romania
[3] Univ Technol Troyes, Int Ctr CVD Innovat Nogent, Pole Technol Sud Champagne, Antenne Nogent, 26 Rue Lavoisier, F-52800 Nogent, France
[4] Univ Bucharest, Fac Chem, Dept Inorgan Chem, 90-92 Panduri Str, Bucharest 050663, Romania
[5] Univ Bucharest, Fac Chem, Res Ctr Catalysts & Catalyt Proc, 4-12 Blv Regina Elisabeta, Bucharest 030018, Romania
关键词
layered double hydroxides; mixed oxides catalysts; transition metal; cobalt; copper; cerium; methane combustion; LAYERED DOUBLE HYDROXIDES; REDOX PROPERTIES; CERIA CATALYSTS; LOW-TEMPERATURE; ANIONIC CLAYS; CU; XPS; CO; HYDROTALCITES; COMBUSTION;
D O I
10.3390/catal10060613
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
To improve the catalytic performance of an active layered double hydroxide (LDH)-derived CuCeMgAlO mixed oxide catalyst in the total oxidation of methane, it was promoted with different transition-metal cations. Thus, two series of multicationic mixed oxides were prepared by the thermal decomposition at 750 degrees C of their corresponding LDH precursors synthesized by coprecipitation at constant pH of 10 under ambient atmosphere. The first series of catalysts consisted of four M(3)CuCeMgAlO mixed oxides containing 3 at.% M (M = Mn, Fe, Co, Ni), 15 at.% Cu, 10 at.% Ce (at.% with respect to cations), and with Mg/Al atomic ratio fixed to 3. The second series consisted of four Co(x)CuCeMgAlO mixed oxides withx= 1, 3, 6, and 9 at.% Co, while keeping constant the Cu and Ce contents and the Mg/Al atomic ratio. All the mixed oxides were characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM) coupled with X-ray energy dispersion analysis (EDX), X-ray photoelectron spectroscopy (XPS), nitrogen adsorption-desorption at -196 degrees C, temperature-programmed reduction under hydrogen (H-2-TPR), and diffuse reflectance UV-VIS spectroscopy (DR UV-VIS), while thermogravimetric and differential thermal analyses (TG-DTG-DTA) together with XRD were used for the LDH precursors. The catalysts were evaluated in the total oxidation of methane, a test reaction for volatile organic compounds (VOC) abatement. Their catalytic performance was explained in correlation with their physicochemical properties and was compared with that of a reference Pd/Al(2)O(3)catalyst. Among the mixed oxides studied, Co(3)CuCeMgAlO was found to be the most active catalyst, with a temperature corresponding to 50% methane conversion (T-50) of 438 degrees C, which was only 19 degrees C higher than that of a reference Pd/Al(2)O(3)catalyst. On the other hand, this T(50)value was ca. 25 degrees C lower than that observed for the unpromoted CuCeMgAlO system, accounting for the improved performance of the Co-promoted catalyst, which also showed a good stability on stream.
引用
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页数:24
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