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Steam reforming of toluene as a biomass tar model compound over CeO_2 promoted Ni/CaO-Al_2O_3 catalytic systems

机译:CeO_2促进Ni / CaO-Al_2O_3催化体系上甲苯蒸汽重整为生物质焦油模型化合物

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Steam reforming of toluene as a biomass tar model compound was performed over Ni supported CaO-Al_2O_3 (Ca-Al) and CeO_2 promoted CaO-Al_2O_3 (Ca-Al-Ce) catalysts to explore promotional effect of CeO_2 on Ca-Al support. Among all the catalysts tested, Ni/Ca -Al-Ce(0.2) catalyst gave superior catalytic performance over other catalysts. The basic strength of catalytic supports measured by CO_2 TPD and Hammett indicator methods indicates Ca-Al-Ce(0.2) support has higher surface basicity and base strength compared to Ca-Al and other Ca-Al-Ce(x) supports. Furthermore, CO pulse chemisorption results showed that Ni/Ca-Al-Ce(0.2) catalyst has a higher amount of surface metallic nickel compared to other Ni/Ca-Al-Ce catalysts. TPR analysis reveals that the redox property of CeO_2 can enhance the reducibility of supported nickel species, which is further confirmed using XPS analysis, where addition of CeO_2 enhanced the interaction of Ni species with Ce by reducing the interaction of Ni species with the Al support, resulting in the formation of Ni° rich surface. However, formation of bulk NiO species was also observed for the catalyst having higher amount of CeO_2. TGA analysis on spent catalysts reveals that all CeO_2-containing catalysts generally result in lower carbon formation rates as compared to Ni/Ca -Al catalyst.
机译:在Ni负载的CaO-Al_2O_3(Ca-Al)和CeO_2促进的CaO-Al_2O_3(Ca-Al-Ce)催化剂上进行甲苯的蒸汽重整,作为生物质焦油模型化合物,以探索CeO_2对Ca-Al载体的促进作用。在所有测试的催化剂中,Ni / Ca -Al-Ce(0.2)催化剂比其他催化剂具有更高的催化性能。通过CO_2 TPD和Hammett指示剂方法测得的催化载体的基本强度表明,与Ca-Al和其他Ca-Al-Ce(x)载体相比,Ca-Al-Ce(0.2)载体具有更高的表面碱度和碱强度。此外,CO脉冲化学吸附结果表明,与其他Ni / Ca-Al-Ce(0.2)催化剂相比,Ni / Ca-Al-Ce(0.2)催化剂具有更高的表面金属镍含量。 TPR分析表明,CeO_2的氧化还原特性可以增强负载型镍物种的还原性,这一点通过XPS分析得到进一步证实,其中XPS分析表明,通过减少Ni物种与Al载体的相互作用,添加CeO_2可以增强Ni物种与Ce的相互作用,导致形成富Ni°的表面。但是,对于具有较高CeO_2含量的催化剂,也观察到大量NiO物质的形成。对废催化剂的TGA分析表明,与Ni / Ca-Al催化剂相比,所有含CeO_2的催化剂通常导致较低的碳形成速率。

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