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Elucidation of metal and support effects during ethanol steam reforming over Ni and Rh based catalysts supported on (CeO2)-ZrO2-La2O3
Catalysis Today ( IF 5.2 ) Pub Date : 2020-03-16 , DOI: 10.1016/j.cattod.2020.03.020
Marinela D. Zhurka , Angeliki A. Lemonidou , Panagiotis N. Kechagiopoulos

Hydrogen production via steam reforming of biomass derived oxygenates is a promising environmental alternative to the use of fossil fuels. The ethanol steam reforming reaction is investigated over Ni and Rh based catalysts supported on ZrO2-La2O3 and CeO2-ZrO2-La2O3 mixed oxides, aiming at the elucidation of the role of the metal and the support in the reaction mechanism. Rh versus Ni is shown to be highly active and more selective with no methane production under all conditions studied. CeO2-ZrO2-La2O3 versus ZrO2-La2O3 is shown to promote efficiently the water gas shift reaction, enhancing hydrogen production substantially. Time on stream studies show that the catalysts on ceria containing supports are highly stable, whereas a gradual deactivation was more evident on the ZrO2-La2O3 supported catalysts. TPO analysis of spent catalysts revealed extremely low amounts of graphitic coke deposited on the Rh catalysts. On Ni, and particularly the ZrO2-La2O3 supported catalyst, larger peaks corresponding to both amorphous and graphitic coke were evident, amounting to higher coke production. The combined effects of metal and support make the catalysts on CeO2-ZrO2-La2O3 most suitable for the reaction, with Rh/CeO2-ZrO2-La2O3 showing particularly high activity, selectivity and stability, with minimal CH4 and CO production resulting at the highest H2 yield.



中文翻译:

阐明在负载于(CeO 2)-ZrO 2 -La 2 O 3上的Ni和Rh基催化剂上进行乙醇蒸汽重整期间的金属和载体效应

通过蒸汽重整生物质衍生的含氧化合物来生产氢是使用化石燃料的有前途的环境替代方案。研究了负载在ZrO 2 -La 2 O 3和CeO 2 -ZrO 2 -La 2 O 3混合氧化物上的Ni和Rh基催化剂的乙醇水蒸气重整反应,旨在阐明金属和载体的作用。反应机理。在所有研究的条件下,Rh对Ni都显示出很高的活性,并且选择性更高,且没有甲烷产生。CeO 2 -ZrO 2 -La 2 O 3与ZrO 2 -La示出了2 O 3可以有效地促进水煤气变换反应,从而显着提高氢气的产生。运转时间研究表明,含二氧化铈载体上的催化剂是高度稳定的,而ZrO 2 -La 2 O 3载体上的催化剂则逐渐失活。用过的催化剂的TPO分析表明,沉积在Rh催化剂上的石墨焦炭极少。在Ni上,特别是在ZrO 2 -La 2 O 3担载的催化剂上,明显的峰对应于无定形和石墨焦炭,这意味着更高的焦炭产量。金属和载体的共同作用使催化剂成为CeO最适合该反应的2 -ZrO 2 -La 2 O 3,其中Rh / CeO 2 -ZrO 2 -La 2 O 3表现出特别高的活性,选择性和稳定性,最小的CH 4和CO生成和最高的H 2屈服。

更新日期:2020-03-16
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