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Syngas production from dry reforming of methane over ni/perlite catalysts: Effect of zirconia and ceria impregnation

机译:Ni /珍珠岩催化剂上甲烷干重整制合成气:氧化锆和二氧化铈浸渍的影响

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Ni catalysts with nominal loadings ranging between 2.5 and 20 wt% were synthesized over perlite by wet impregnation, then filtered, washed and calcined at 500 degrees C. Chemical analyses performed by MP-AES revealed that the maximum Ni content loaded over perlite corresponded to similar to 15 wt%. Therefore, for comparison reasons, a Ni(20 wt%)/perlite catalyst was prepared by wetness impregnation without performing any washing treatment. The so prepared catalysts were tested in methane dry reforming without performing any pretreatment reduction. The catalytic performances were compared by increasing the temperature from 500 up to 800 degrees C under the reaction mixture composed of 15 vol% CH4 + 15 vol% CO2/N-2. Ni(15 wt%)/perlite was the most active catalyst among the series of monometallic samples. The effect of co-impregnating perlite with Ni and Zr or Ni and Ce precursors in order to obtain catalysts with final composition, Ni(15 wt%), 10 and 20 wt% as Zr or Ce, perlite (75 or 65 wt%) was, then, investigated. Characterizations performed by XRD, BET, DRS and H-2-TPR evidenced that the physico-chemical and reduction properties are influenced by the Ni content and by the presence of zirconia and ceria oxides. It is worth of noting the increased reducibility of NiO species promoted by zirconia and ceria addition. The catalytic activity in the dry reforming of methane was also affected by the presence of doping oxides, in terms of enhanced CH4 and CO2 conversions and higher H-2/CO atomic ratios. Runs tests at 700 degrees C for 12 h were carried out and the spent catalysts were analysed by TGA and TEM. Over Ni(15 wt%)/perlite large amount of amorphous carbon grows on the surface blocking the active centres, while zirconia and ceria doping improved the resistance to carbon poisoning favouring growing of filamentous carbon residues in small amount. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
机译:通过湿法浸渍在珍珠岩上合成名义负载量在2.5至20 wt%之间的Ni催化剂,然后在500摄氏度下过滤,洗涤和煅烧。MP-AES进行的化学分析表明,负载在珍珠岩上的最大Ni含量相当于至15重量%。因此,出于比较的原因,在不进行任何洗涤处理的情况下通过湿润浸渍制备了Ni(20wt%)/珍珠岩催化剂。在不进行任何预处理还原的情况下,将如此制备的催化剂在甲烷干重整中进行测试。通过在由15体积%CH 4 +15体积%CO 2 / N-2组成的反应混合物下将温度从500℃升高至800℃来比较催化性能。 Ni(15 wt%)/珍珠岩是一系列单金属样品中活性最高的催化剂。用Ni和Zr或Ni和Ce前驱体共浸渍珍珠岩以获得最终成分为Ni(15 wt%),10和20 wt%Zr或Ce珍珠岩(75或65 wt%)的催化剂的效果然后进行了调查。 XRD,BET,DRS和H-2-TPR进行的表征表明,理化性质和还原性质受Ni含量以及氧化锆和二氧化铈的存在的影响。值得注意的是,氧化锆和二氧化铈的添加促进了NiO物种的还原性。甲烷干重整中的催化活性还受到掺杂氧化物的存在的影响,就提高了CH4和CO2的转化率以及提高了H-2 / CO原子比而言。在700摄氏度下进行了12小时的运行测试,并通过TGA和TEM分析了废催化剂。超过Ni(15 wt%)/珍珠岩,大量无定形碳在阻止活性中心的表面生长,而氧化锆和二氧化铈掺杂改善了对碳中毒的抵抗力,有利于少量丝状碳残留物的生长。 (C)2018氢能出版物有限公司。由Elsevier Ltd.出版。保留所有权利。

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