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Aqueous-phase reforming of renewables for selective hydrogen production in the presence of supported platinum catalysts

机译:在负载型铂催化剂存在下,可再生能源进行水相重整以选择性生产氢气

摘要

The evolution of our society is impossible without a constant progress in life-important areas such as chemical engineering and technology. Innovation, creativity and technology are three main components driving the progress of chemistry further towards a sustainable society. Biomass, being an attractive renewable feedstock for production of fine chemicals, energy-rich materials and even transportation fuels, captures progressively new positions in the area of chemical technology. Knowledge of heterogeneous catalysis and chemical technology applied to transformation of biomass-derived substances will open doors for a sustainable economy and facilitates the discovery of novel environmentally-benign processes which probably will replace existing technologies in the era of biorefinary.Aqueous-phase reforming (APR) is regarded as a promising technology for production of hydrogen and liquids fuels from biomass-derived substances such as C3-C6 polyols. In the present work, aqueous-phase reforming of glycerol, xylitol and sorbitol was investigated in the presence of supported Pt catalysts. The catalysts were deposited on different support materials, including Al2O3, TiO2 and carbons. Catalytic measurements were performed in a laboratory-scale continuous fixedbed reactor. An advanced analytical approach was developed in order to identify reaction products and reaction intermediates in the APR of polyols. The influence of the substrate structure on the product formation and selectivity in the APR reaction was also investigated, showing that the yields of the desired products varied depending on the substrate chain length. Additionally, the influence of bioethanol additive in the APR of glycerol and sorbitol was studied. A reaction network was advanced explaining the formation of products and key intermediates. The structure sensitivity in the aqueous-phase reforming reaction was demonstrated using a series of platinum catalysts supported on carbon with different Pt cluster sizes in the continuous fixed-bed reactor. Furthermore, a correlation between texture physico-chemical properties of the catalysts and catalytic data was established. The effect of the second metal (Re, Cu) addition to Pt catalysts was investigated in the APR of xylitol showing a superior hydrocarbon formation on PtRe bimetallic catalysts compared to monometallic Pt. On the basis of the experimental data obtained, mathematical modeling of the reaction kinetics was performed. The developed model was proven to successfully describe experimental data on APR of sorbitol with good accuracy.
机译:没有在诸如化学工程和技术等重要生命领域中不断取得进步,我们的社会就不可能发展。创新,创造力和技术是推动化学向可持续社会发展的三个主要组成部分。生物质是一种有吸引力的可再生原料,用于生产精细化学品,高能材料甚至运输燃料,在化学技术领域逐渐占据了新的位置。多相催化和化学技术应用于生物质衍生物质转化的知识将为可持续的经济打开一扇门,并促进发现新的环境友好方法,这些方法可能将替代生物精炼时代的现有技术。 )被认为是一种由生物质衍生的物质(例如C3-C6多元醇)生产氢和液体燃料的有前途的技术。在本工作中,研究了在负载的Pt催化剂存在下甘油,木糖醇和山梨糖醇的水相重整。催化剂沉积在不同的载体材料上,包括Al2O3,TiO2和碳。催化测量在实验室规模的连续固定床反应器中进行。为了鉴定多元醇APR中的反应产物和反应中间体,开发了一种先进的分析方法。还研究了底物结构对APR反应中产物形成和选择性的影响,表明所需产物的产率随底物链长而变化。此外,研究了生物乙醇添加剂对甘油和山梨糖醇APR的影响。建立了反应网络,解释了产物和关键中间体的形成。在连续固定床反应器中,使用负载在具有不同Pt簇尺寸的碳上的一系列铂催化剂证明了水相重整反应中的结构敏感性。此外,建立了催化剂的织构理化性质与催化数据之间的相关性。在木糖醇的APR中研究了向Pt催化剂中添加第二种金属(Re,Cu)的效果,与单金属Pt相比,在PtRe双金属催化剂上形成的碳氢化合物更好。根据获得的实验数据,对反应动力学进行数学建模。实践证明,所开发的模型可以成功地准确描述山梨醇APR的实验数据。

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    Kirilin Alexey;

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  • 年度 2013
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  • 正文语种 en
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