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添加 CeO₂ 对 Al₂O₃ 负载的 Pt 催化剂在甘油水相重整反应中的影响。

Effect of CeO₂ addition to Al₂O₃ supports for Pt catalysts on the aqueous-phase reforming of glycerol.

机构信息

School of Chemical and Biomolecular Engineering, University of Sydney, Sydney, NSW, 2006, Australia.

出版信息

ChemSusChem. 2013 Jun;6(6):1006-13. doi: 10.1002/cssc.201200797. Epub 2013 Apr 24.

DOI:10.1002/cssc.201200797
PMID:23616477
Abstract

A series of Pt catalysts supported on Al₂O₃ that was doped with different amounts of CeO₂ was developed, characterized, and tested in the aqueous-phase reforming (APR) of glycerol to H₂. Catalyst 3Pt/3CeAl, which bore 3 wt% Pt on a support that contained 3 wt % CeO₂, showed the highest carbon conversion to gas (85%) and the highest H₂ yield (80%) for a feedstock of 1 wt% glycerol in water at 240 °C and 40 bar. A CeO₂/Al₂O₃ support with only 1 wt% Pt also showed high H₂ selectivity and carbon conversion to gas, as well as a much lower CH₄ yield than the benchmark 3Pt/Al catalyst, clearly demonstrating that doping the support with 3 wt% CeO2 improved the APR of glycerol. H₂ chemisorption results showed that the highest metal dispersion (58%) and active surface area (4.3 m(2)g(-1)) were achieved for the support that contained 3 wt% CeO₂, and this effect appeared to be primarily responsible for the high H₂ yield and carbon conversion to gas. No CO was observed in the product gas; therefore, this gas could potentially be used directly in proton exchange membrane fuel cells. Thus, including CeO₂ in the Al₂O₃ catalyst support enhanced both the activity and selectivity towards H₂ of a Pt catalyst for the APR of glycerol.

摘要

开发了一系列负载不同量 CeO₂的 Al₂O₃ 负载 Pt 催化剂,并对其进行了表征和测试,用于甘油在水相重整(APR)制氢。在 240°C 和 40 bar 下,对于 1 wt%甘油在水中的进料,负载 3 wt% Pt 的催化剂 3Pt/3CeAl 显示出最高的碳转化率为气体(85%)和最高的 H₂产率(80%)。CeO₂/Al₂O₃ 载体中仅负载 1 wt% Pt 的催化剂也表现出高的 H₂选择性和碳转化率为气体,以及比基准 3Pt/Al 催化剂低得多的 CH₄产率,这清楚地表明,在载体中掺杂 3 wt% CeO₂ 可以提高甘油的 APR。H₂化学吸附结果表明,在含有 3 wt% CeO₂ 的载体上实现了最高的金属分散度(58%)和比表面积(4.3 m²g⁻¹),这种效果似乎主要是导致高 H₂产率和碳转化率为气体的原因。在产物气中未观察到 CO;因此,这种气体可直接用于质子交换膜燃料电池。因此,在 Al₂O₃ 催化剂载体中包含 CeO₂ 可增强 Pt 催化剂对甘油 APR 的 H₂活性和选择性。

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