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Catalytic assessment of a Ni-La-Sn ternary metallic system in ethanol steam reforming and the influence of the Sn/La atomic ratio in the catalytic performance

机译:乙醇蒸汽重整中Ni-La-Sn三元金属体系的催化评估及Sn / La原子比在催化性能下的影响

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Nickel based catalysts (15 wt.%) supported on a La-Sn mixed oxides (Sn/La atomic ratio = 1, 0.75, 0.5, 0.25 and 0) were prepared by a coprecipitation technique involving pH adjustment with KOH and then calcined at 950 degrees C. XRD analysis of the catalysts containing Sn showed the presence of the pyrochlore-like phase La2Sn2O7 and an intermetallic NixSny compounds as active phase. For the Sn/La ratios lower than 1, the formation of the perovskite-like phases La2NiSnO6 and LaNiO3 was also observed, with relative amounts in weight dependent of the Sn/La ratio, although they were easily destroyed under reaction conditions to form a more Sn-rich active phase. All the catalysts were active in the ethanol steam reforming at 650 degrees C with a production of a H2 and CO2 rich gas mixture. While the Sn presence in the catalyst decreases its catalytic activity, the formation of an intermetallic NixSny phase increases its resistance to the formation of carbonaceous residues and the presence of Sn+4 species in the pyrochlore compound promotes the WGSR decreasing the CO production. Carbonaceous residues on the spent catalysts were analyzed by TGA, EDS, Elemental Analysis and Raman Spectroscopy showing differences in their quantity and nature depending on the Sn/La ratio.
机译:采用共沉淀技术制备了负载在La-Sn混合氧化物(Sn/La原子比=1,0.75,0.5,0.25和0)上的镍基催化剂(15 wt.%),该技术涉及用KOH调节pH值,然后在950℃下煅烧。对含Sn催化剂的XRD分析表明,存在类似焦绿石的La2Sn2O7相和作为活性相的金属间化合物NixSny。当Sn/La比低于1时,还观察到类钙钛矿相La2NiSnO6和LaNiO3的形成,其相对量取决于Sn/La比,尽管它们在反应条件下很容易被破坏以形成更富Sn的活性相。所有的催化剂都在650℃的乙醇蒸汽重整反应中表现出活性,生成了富含H2和CO2的混合气体。虽然催化剂中的Sn降低了其催化活性,但金属间化合物NixSny相的形成增加了其抗碳质残留物形成的能力,并且焦绿石化合物中Sn+4物种的存在促进了WGSR降低了CO的生成。通过TGA、EDS、元素分析和拉曼光谱对废催化剂上的含碳残留物进行了分析,表明它们的数量和性质因Sn/La比率而异。

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