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Hydrogen production by glycerol steam reforming over SBA-15-supported nickel catalysts: Effect of alkaline earth promoters on activity and stability

机译:SBA-15负载的镍催化剂上甘油蒸汽重整制氢:碱土助催化剂对活性和稳定性的影响

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Mg- and Ca-modifled Ni/SBA-15 catalysts were prepared by incipient wetness impregnation (7 wt% Ni) to be studied for catalytic glycerol steam reforming at 600 °C High space velocities were selected in order to highlight differences in activity between catalysts and deactivation effects at relatively short time. Characterization of the calcined, reduced and used samples was carried out by XRD, 1CP-AES, N2-physisorption, TGA, H2-TPR, TEM and HCNS elemental analysis. XRD and TEM demonstrated dispersing effect of Mg and Ca on the Ni phase, while TPR evidenced strengthening of the Ni-support interaction by Mg and Ca incorporation to the Ni/SBA-15 catalyst. These effects were significantly noticeable in the Ni/Ca/SBA-15 sample. As a consequence, the Ni/Ca/SBA-15 catalyst achieved the highest glycerol conversion (98.4%) and yield to gases formation (69.9 wt%) with a hydrogen content of 53 vol%. Additionally, this catalyst was stable with time on stream under glycerol steam reforming and showed the lowest coke deposition. This was ascribed to the formation of highly defective carbon deposits, easier to be gasified under reaction conditions, mainly in the form of non-encapsulating carbon nanofibres formed on the small and strongly-supported Ni particles.
机译:Mg和Ca改性的Ni / SBA-15催化剂通过初湿浸渍(7 wt%Ni)制备,用于研究600°C的甘油催化蒸汽重整,选择高空速以突出催化剂之间的活性差异。以及在相对较短的时间内失效。通过XRD,1CP-AES,N2-物理吸附,TGA,H2-TPR,TEM和HCNS元素分析对煅烧,还原和使用的样品进行表征。 XRD和TEM证实了Mg和Ca在Ni相上的分散作用,而TPR表明通过将Mg和Ca掺入Ni / SBA-15催化剂中可以增强Ni-载体的相互作用。在Ni / Ca / SBA-15样品中,这些影响非常明显。结果,Ni / Ca / SBA-15催化剂实现了最高的甘油转化率(98.4%)和具有53vol%的氢含量的生成气体的产率(69.9wt%)。另外,该催化剂在甘油蒸汽重整下随时间流逝是稳定的,并且显示出最低的焦炭沉积。这归因于高度缺陷的碳沉积物的形成,该碳沉积物在反应条件下更容易被气化,主要形式是在小且强支撑的Ni颗粒上形成的非包封碳纳米纤维。

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