Ni/Al2O3 promoted by CeO2, CeO2-La2O3, and CeO2-ZrO2 supported on cordierite monoliths for methane steam reforming

IF 5.2 2区化学 Q1 CHEMISTRY, APPLIED Catalysis Today Pub Date : 2024-10-24 DOI:10.1016/j.cattod.2024.115107

Victória Gonçalves F Pereira , Ana Serrano-Lotina , Raquel Portela , Miguel A. Bañares , Clarissa Perdomo Rodrigues , Fabio Souza Toniolo

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Abstract

Promotion of Ni-based catalysts supported on cordierite monoliths was investigated for methane steam reforming. First, cordierite was coated by ɣ-Al₂O_3, and then the catalyst components were deposited by successive wet impregnation, obtaining: NiAl/cordierite; NiCeAl/cordierite; NiCeLaAl/cordierite and NiCeZrAl/cordierite. The monolithic catalysts were characterized by adherence test, Scanning Electron Microscopy with Energy-Dispersive X-ray Spectroscopy (SEM-EDX), N₂ physisorption, Temperature-Programmed Reduction (TPR), CO chemisorption, as well as by in situ and operando Raman spectroscopy. The catalyst layer showed very good adherence and distribution of the components over the cordierite surface. The catalysts presented high activity between 600 and 800 °C at a H₂O/CH₄ molar ratio=1.5, except for NiCeAl/cordierite, which obtained lower methane conversion, associated with its lower nickel dispersion. The catalysts showed high stability under extreme conditions for carbon deposition (600 °C and H₂O/CH₄=1), over 90 h on stream. Raman spectroscopy revealed the presence of oxygen vacancies, which may be increased during ceria reduction, highlighting the potential of these catalysts to enhance the resistance to deactivation by carbon deposition in long-term tests.

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以堇青石整体柱为支撑的 CeO2、CeO2-La2O3 和 CeO2-ZrO2 促进 Ni/Al2O3 用于甲烷蒸汽转化

研究了堇青石整体支撑的镍基催化剂对甲烷蒸汽转化的促进作用。首先用ɣ-Al2O3 对堇青石进行包覆，然后通过连续湿法浸渍沉积催化剂组分，得到了NiAl/堇青石、NiCeAl/堇青石、NiCeLaAl/堇青石和 NiCeZrAl/堇青石。通过附着力测试、扫描电子显微镜与能量色散 X 射线光谱（SEM-EDX）、N2 物理吸附、温度编程还原（TPR）、CO 化学吸附以及原位和操作拉曼光谱，对整体催化剂进行了表征。催化剂层在堇青石表面显示出非常好的附着性和组分分布。在 H2O/CH4 摩尔比=1.5 的条件下，催化剂在 600 至 800 °C 之间表现出较高的活性，但 NiCeAl/cordierite 除外，其甲烷转化率较低，这与其镍分散度较低有关。在碳沉积的极端条件下（600 °C，H2O/CH4=1），催化剂在90小时内显示出很高的稳定性。拉曼光谱显示存在氧空位，这可能在铈还原过程中增加，突出了这些催化剂在长期测试中提高抗碳沉积失活能力的潜力。

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来源期刊

Catalysis Today 化学-工程：化工

CiteScore

11.50

自引率

3.80%

发文量

573

审稿时长

2.9 months

期刊介绍： Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues. Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.