Highly active and stable Co (Co3O4)_Sm2O3 nano-crystallites derived from Sm2Co7 and SmCo5 intermetallic compounds in NH3 synthesis and CO2 conversion

被引:0
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作者
Marakatti, Vijaykumar S. [1 ]
Ronda-Lloret, Maria [2 ]
Krajci, Marian [3 ]
Joseph, Boby [4 ]
Marini, Carlo [5 ]
Jose Delgado, Juan [6 ,7 ]
Devred, Francois [1 ]
Raveendran Shiju, N. [2 ]
Gaigneaux, Eric M. [1 ]
机构
[1] Univ Catholique Louvain UCLouvain, Inst Condensed Matter & Nanosci IMCN, Mol Chem Solids & Catalysis MOST, Pl Louis Pasteur, B-1348 Louvain La Neuve, Belgium
[2] Univ Amsterdam, Vant Hoff Inst Mol Sci, Sci Pk 904, NL-1090 GD Amsterdam, Netherlands
[3] Slovak Acad Sci, Inst Phys, SK-84511 Bratislava, Slovakia
[4] Elettra Sincrotrone Trieste SCpA, SS 14,Km 163-5 Area Sci Pk, I-34149 Basovizza, Italy
[5] ALBA Synchrotron Light Source, Carrer Llum 2-26, Barcelona, Spain
[6] Univ Cadiz, Inst Univ Invest Microscopia Elect & Mat, Dept Ciencia Mat & Ingn Metalurg & Quim Inorgan, Puerto Real 11510, Spain
[7] Univ Cadiz, Inst Univ Invest Microscopia Elect & Mat, IMEYMAT, Puerto Real 11510, Spain
基金
欧盟地平线“2020”;
关键词
METAL-SUPPORT INTERACTIONS; MEDIATED NITROGEN TRANSFER; BARIUM-PROMOTED COBALT; AMMONIA-SYNTHESIS; EFFICIENT CATALYST; NANOPARTICLES; HYDROGENATION; ACTIVATION; BUTANE; XAFS;
D O I
10.1039/d1cy01956b
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
Intermetallic compounds (IMCs) are interesting materials in the field of heterogeneous catalysis due to their ordered structure and tunable electronic properties. These IMCs can act as precursor to synthesize metal/metal oxide composite catalysts that are more active than just the starting IMCs. In this work, Sm2Co7 and SmCo5 IMCs were used as precursors to prepare highly active and stable Co_SmO, Co_Sm2O3 and Co3O4_Sm2O3 catalysts via controlled modification. Transmission electron microscopy (TEM) demonstrated that Co and Sm2O3 Nano crystallites were formed after the modification of the IMC. IMCs derived Co_SmO and Co_Sm2O3 were stable and active in NH3 synthesis with very low activation energy of 55 and 77 kJ mol(-1) respectively. The structural, morphological and surface characterization revealed that a strong metal support interaction existed between Co and Sm2O3 (electronic effect) along with the presence of surface steps and edges of Co nano crystallites (structural effect) that activate the N-2 at low temperature (360 degrees C). Similarly, Co3O4_Sm2O3 derived from the IMC were found to exhibit high CO2 and butane conversion in butane dry reforming at low temperature (550 degrees C) with excellent stability. The study revealed that the presence of Co3O4 and Sm2O3 active sites in close proximity (geometrical effect) promoted the simultaneous adsorption or activation of butane and CO2. The Co_Sm2O3 and Co3O4_Sm2O3 derived from IMCs exhibited superior catalytic performance in both NH3 synthesis and butane dry reforming compared to similar compositional catalyst synthesized by hydrothermal route. These studies pave the way to potential uses of IMCs as precursors to derive composite metal/metal oxide catalysts that are highly stable and active despite their low surface areas.
引用
收藏
页码:686 / 706
页数:21
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