Ammonia Decomposition over Iron Phthalocyanine-Based Materials

被引:13
|
作者
Tueysuez, Harun [1 ]
Schueth, Ferdi [1 ]
Zhi, Linjie [2 ]
Muellen, Klaus [2 ]
Comotti, Massimiliano [1 ]
机构
[1] Max Planck Inst Kohlenforsch, Heterogeneous Catalysis Dept, D-45470 Mulheim, Germany
[2] Max Planck Inst Polymer Res, Dept Synthet Chem, D-55128 Mainz, Germany
关键词
ammonia decomposition; carbon; catalyst; iron; pyrolysis; COX-FREE HYDROGEN; CARBON NANOTUBES; NH3; DECOMPOSITION; METAL PHTHALOCYANINES; CATALYTIC-PROPERTIES; RU CATALYST; GENERATION; NANOPARTICLES; STATE; FUEL;
D O I
10.1002/cctc.201500024
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
Iron phthalocyanine-based materials have been used herein as efficient catalysts for the ammonia decomposition reaction. These materials showed high activity, even superior to that showed by the commercial nickel-based catalyst and iron-doped carbon nanotubes, which were used as benchmarks in this study. Catalyst stability under reaction conditions appeared satisfactory, because no deactivation phenomena were observed. The type of the phthalocyanine precursor did not affect the catalytic performance; however, the preparation method had a strong effect. If the resulting material was exposed to the reaction conditions, some structural modification occurred. No clear correlation between phase composition and activity could be established because similar nitrogen content and similar crystalline domains in the sample led to different behaviors. However, the results of extensive characterization suggested that catalytic activities and conversion profiles were most likely dependent on material textural properties and thus on the preparation method used. The accessibility of iron species seems to be limited for catalysts prepared under vacuum. These phenomena are most likely responsible for the activation profile and for the low catalytic activity typical of these materials. In contrast, higher accessibility of iron species, typical of materials prepared under argon, would lead to improved and stable catalytic performance.
引用
收藏
页码:1453 / 1459
页数:7
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