Rahemi Nader, Haghighi Mohammad, Babaluo Ali Akbar, Jafari Mahdi Fallah, Estifaee Pooya
Chemical Engineering Faculty, Sahand University of Technology, PO Box 51335-1996, Sahand New Town, Tabriz, Iran.
J Nanosci Nanotechnol. 2013 Jul;13(7):4896-908. doi: 10.1166/jnn.2013.7585.
Ni/Al2O3 and Ni/Al2O3-CeO2 nanocatalysts have been prepared with impregnation method, treated with non-thermal plasma, characterized and tested for dry reforming of methane. For catalyst characterization, the following techniques have been used: XRD, FESEM, TEM, EDX dot mapping, BET, FTIR, TG-DTG, and XPS techniques. According to XRD and XPS, Ni in all catalysts exists as NiO and NiAl2O4 that existence of NiAl2O4 reveals strong interaction between active phase and support. Catalyst particles had smaller average particle size in plasma treated Ni/Al2O3-CeO2 nanocatalyst with less agglomeration. Homogenous dispersion of active phase, narrower particle size distribution, and uniform morphology has been observed in ceria containing plasma treated catalyst. The plasma treated Ni/Al2O3-CeO2 nanocatalyst showed bigger NiAl2O4/NiO ratio in XPS analysis that is indicative of stronger interaction between Ni and Al2O3 in the presence of CeO2. The dry reforming of methane was carried out at 550-850 degrees C using a mixture of CH4:CO2 (0.5:2). Improved morphology of the plasma treated Ni/Al2O3-CeO2 nanocatalyst, resulted from both CeO2 and plasma treatment, caused higher ability of catalyst in H2 and CO production. Product yield decreased at higher GHSVs, due to the fact that mass transport limitations will be more severe at low residence time, but this reduction would be less noticeable in the plasma treated Ni/Al2O3-CeO2 nanocatalyst. In addition, the plasma treated Ni/Al2O3-CeO2 nanocatalyst can keep the reactivity without deactivation for either CH4 or CO2 conversion better than other investigated catalysts.
采用浸渍法制备了Ni/Al2O3和Ni/Al2O3-CeO2纳米催化剂,用非热等离子体进行处理,对其进行表征并测试甲烷干重整性能。对于催化剂表征,采用了以下技术:XRD、FESEM、TEM、EDX点映射、BET、FTIR、TG-DTG和XPS技术。根据XRD和XPS分析,所有催化剂中的Ni均以NiO和NiAl2O4形式存在,NiAl2O4的存在表明活性相与载体之间存在强相互作用。在经等离子体处理的Ni/Al2O3-CeO2纳米催化剂中,催化剂颗粒的平均粒径较小,团聚较少。在含二氧化铈的经等离子体处理的催化剂中观察到活性相的均匀分散、较窄的粒径分布和均匀的形态。经等离子体处理的Ni/Al2O3-CeO2纳米催化剂在XPS分析中显示出更大的NiAl2O4/NiO比,这表明在CeO2存在下Ni与Al2O3之间的相互作用更强。甲烷干重整在550-850℃下使用CH4:CO2(0.5:2)的混合物进行。CeO2和等离子体处理共同作用导致经等离子体处理的Ni/Al2O3-CeO2纳米催化剂形态改善,使其在H2和CO生成方面具有更高的催化能力。在较高的气体时空速下产物产率降低,这是因为在低停留时间下传质限制会更严重,但这种降低在经等离子体处理的Ni/Al2O3-CeO2纳米催化剂中不太明显。此外,经等离子体处理的Ni/Al2O3-CeO2纳米催化剂在CH4或CO2转化方面比其他研究的催化剂能更好地保持反应活性而不发生失活。