Influence of lanthanum stoichiometry in La1-xFeO3-δ perovskites on their structure and catalytic performance in CH4 total oxidation

被引:104
作者
Faye, Jeremy [1 ,2 ]
Baylet, Alexandre [2 ]
Trentesaux, Martine [1 ]
Royer, Sebastien [2 ,3 ]
Dumeignil, Franck [1 ,4 ]
Duprez, Daniel [2 ,3 ]
Valange, Sabine [2 ,3 ]
Tatibouet, Jean-Michel [2 ,3 ]
机构
[1] Univ Lille Nord France, UMR CNRS 8181, Unite Catalyse & Chim Solide, F-59655 Villeneuve Dascq, France
[2] Univ Poitiers, Catalyse Chim Organ Lab, CNRS UMR 6503, F-86022 Poitiers, France
[3] Univ Poitiers, Inst Chim Milieux & Mat Poitiers IC2MP, CNRS UMR 7285, Ecole Natl Super Ingn Poitiers, F-86022 Poitiers, France
[4] Inst Univ France, F-75005 Paris, France
关键词
CH4 total oxidation; Non-stoichiometric perovskite; XPS; Redox properties; Iron oxide; NONSTOICHIOMETRIC LAFEO3 PEROVSKITE; A-SITE CATION; METHANE COMBUSTION; SURFACE-PROPERTIES; CO OXIDATION; MIXED OXIDES; LAMO3; OXIDES; IRON-OXIDES; TEMPERATURE; OXYGEN;
D O I
10.1016/j.apcatb.2012.07.001
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
A series of iron-based La1-xFeO3-delta perovskites (with x = 0, 0.1, 0.2, 0.3 and 0.4) was prepared by the so-called self-combustion method using glycine as an ignition promoter. The chemical, structural and surface properties of these mixed oxides were thoroughly characterized before the determination of their activity in the total oxidation of methane. The catalytic data indicated a strong dependence of the methane conversion towards the catalyst elemental composition. A progressive Fe2O3 enrichment of the perovskite surface was clearly evidenced by XPS characterization when decreasing the lanthanum content of the solid. Such additional undesirable surface iron oxide induced an inhibiting effect on the catalytic activity. As a result, while the La1-xFeO3-delta (x = 0, 0.1, 0.2, 0.3, 0.4) perovskites presented moderated performances in methane total oxidation, the most efficient lanthanum iron-based perovskite is the stoichiometric LaFeO3 mixed-oxide that exhibits the most adapted surface and global composition, resulting in a CH4 conversion of 86% at 873 K. (c) 2012 Elsevier B.V. All rights reserved.
引用
收藏
页码:134 / 143
页数:10
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