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H2 from biofuels and carriers: gas-phase and surface ethanol conversion pathways on Rh/Al2O3 investigated by annular microreactor coupled with Raman and FTIR spectroscopy
Journal of Catalysis ( IF 7.3 ) Pub Date : 2022-06-21 , DOI: 10.1016/j.jcat.2022.06.012
Veronica Piazza , Roberto B.S. Junior , Giulia Luccisano , Daniela Pietrogiacomi , Gianpiero Groppi , Delia Gazzoli , Alessandra Beretta

Catalytic Partial Oxidation (CPO) and Steam Reforming of ethanol are studied on Rh/Al2O3. The main goal of the work is the development of a comprehensive methodological approach coupling catalytic activity testing and surface characterization, in order to investigate both ethanol-to-H2 conversion pathways and C-deposits formation.

Experiments are performed in an annular reactor and four reaction regimes in CPO are identified: ethanol oxidative dehydrogenation to acetaldehyde (T < 200 °C); total oxidation and initial ethanol O2-assisted ethanol decomposition (200 °C < T < 300 °C); early H2 and CO production for reforming of surface CHx fragments (300 °C < T < 500 °C); development of ethanol steam reforming (T > 500 °C).

Adsorbed species and C-deposits are characterized via operando FTIR, ex-situ Raman and TPO. These analyses proved that the different reaction regimes are reflected in continuous changes of catalytic surface coverage, passing from the co-existence of ethanol and O2 at low temperature, to wide C-coverage when O2 is consumed. At 700 °C gasification is favoured and promotes surface cleaning.



中文翻译:

来自生物燃料和载体的 H2:环形微反应器结合拉曼和 FTIR 光谱研究 Rh/Al2O3 上的气相和表面乙醇转化途径

在Rh/Al 2 O 3上研究了乙醇的催化部分氧化(CPO)和蒸汽重整。这项工作的主要目标是开发一种将催化活性测试和表面表征相结合的综合方法,以研究乙醇到 H 2的转化途径和碳沉积物的形成。

实验在环形反应器中进行,确定了 CPO 中的四种反应方案:乙醇氧化脱氢制乙醛(T < 200 °C);总氧化和初始乙醇 O 2辅助乙醇分解 (200 °C < T < 300 °C);用于重整表面 CH x碎片的早期 H 2和 CO 生产(300 °C < T < 500 °C);开发乙醇蒸汽重整 (T > 500 °C)。

通过操作 FTIR、异位拉曼和 TPO表征吸附的物质和 C-沉积物。这些分析证明,不同的反应方式反映在催化表面覆盖率的连续变化上,从低温下乙醇和O 2的共存到消耗O 2时的宽C覆盖率。在 700 °C 时,气化是有利的并促进表面清洁。

更新日期:2022-06-21
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