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由甘油蒸汽重整制取可再生氢气:La2O3 和 CeO2 对 Pt/Al2O3 催化剂的影响。

Renewable H2 from glycerol steam reforming: effect of La2O3 and CeO2 addition to Pt/Al2O3 catalysts.

机构信息

Department of Chemical Sciences, ICCOM-CNR Research Unit, University of Trieste via L. Giorgieri 1, 34127 Trieste, Italy.

出版信息

ChemSusChem. 2010 May 25;3(5):619-28. doi: 10.1002/cssc.200900243.

Abstract

Glycerol is the main byproduct of biodiesel production and its increased production volume derives from the increasing demand for biofuels. The conversion of glycerol to hydrogen-rich mixtures presents an attractive route towards sustainable biodiesel production. Here we explored the use of Pt/Al(2)O(3)-based catalysts for the catalytic steam reforming of glycerol, evidencing the influence of La(2)O(3) and CeO(2) doping on the catalyst activity and selectivity. The addition of the latter metal oxides to a Pt/Al(2)O(3) catalyst is found to significantly improve the glycerol steam reforming, with high H(2) and CO(2) selectivities. A good catalytic stability is achieved for the Pt/La(2)O(3)/Al(2)O(3) system working at 350 degrees C, while the Pt/CeO(2)/Al(2)O(3) catalyst sharply deactivates after 20 h under similar conditions. Studies carried out on fresh and exhausted catalysts reveal that both systems maintain high surface areas and high Pt dispersions. Therefore, the observed catalyst deactivation can be attributed to coke deposition on the active sites throughout the catalytic process and only marginally to Pt nanoparticle sintering. This work suggests that an appropriate support composition is mandatory for preparing high-performance Pt-based catalysts for the sustainable conversion of glycerol into syngas.

摘要

甘油是生物柴油生产的主要副产物,其产量的增加源于生物燃料需求的增加。将甘油转化为富含氢气的混合物是一种很有吸引力的可持续生物柴油生产途径。在这里,我们探索了基于 Pt/Al(2)O(3)的催化剂在甘油催化蒸汽重整中的应用,证明了 La(2)O(3)和 CeO(2)掺杂对催化剂活性和选择性的影响。将后两种金属氧化物添加到 Pt/Al(2)O(3)催化剂中,发现可以显著提高甘油蒸汽重整的效果,同时具有较高的 H(2)和 CO(2)选择性。在 350°C 下工作的 Pt/La(2)O(3)/Al(2)O(3)体系具有良好的催化稳定性,而在相似条件下,Pt/CeO(2)/Al(2)O(3)催化剂在 20 小时后急剧失活。对新鲜和废弃催化剂的研究表明,这两种体系都保持着较高的比表面积和较高的 Pt 分散度。因此,观察到的催化剂失活可以归因于在整个催化过程中活性位上积碳的沉积,而不是 Pt 纳米颗粒的烧结。这项工作表明,对于将甘油可持续地转化为合成气,制备高性能的 Pt 基催化剂,适当的载体组成是必不可少的。

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