Activity and stability of powder and monolith-coated Ni/GDC catalysts for CO2 methanation
Activity and stability of powder and monolith-coated Ni/GDC catalysts for CO2 methanation
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DOI：
10.1016/j.apcatb.2017.12.078
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发表时间：
2018-06
期刊：
影响因子：
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通讯作者：
A. Vita;C. Italiano;L. Pino;P. Frontera;M. Ferraro;V. Antonucci
中科院分区：
文献类型：
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作者：
A. Vita;C. Italiano;L. Pino;P. Frontera;M. Ferraro;V. Antonucci
通过Sabatier工艺的CO2甲烷化正在获得电力到天然气（P2 G）应用的兴趣。在这项工作中，在大气压下改变反应温度（TSET= 300-600 °C）和空速（GHSV = 10，000 - 50，000 h-1），研究了Ni/GDC（钆掺杂的氧化铈）催化剂上的CO2甲烷化活性和稳定性。具有不同Ni含量（15-50重量%）的粉末催化剂采用溶液燃烧合成法（SCS）合成了1，2，4-二羟基苯甲酸甲酯。采用相同的方法原位沉积Ni/GDC（50 wt.% Ni）涂层（500 cpsi）。采用N2吸附-脱附、X射线衍射（XRD）、H2程序升温还原（H2-TPR）、CO2程序升温脱附（CO2-TPD）、X射线光电子能谱（XPS）、透射电子显微镜（TEM）和扫描电子显微镜（SEM）对催化剂进行了表征。讨论了结构化催化床沿着的温度分布来解释实验结果。由于金属与载体的相互作用、碱性和氧空位的增强，催化性能随着Ni含量的增加而提高。通过完全可重复的SCS方法，在堇青石单块上原位沉积均匀、薄且高电阻的催化层。结构化催化剂由于同时具有低催化剂负载和高流速而显示出每单位重量催化剂的高甲烷产率。在200小时的运行时间内观察到优异的稳定性。本文的研究结果指出了在结构化催化剂上实现CO2甲烷化的重要方面，为进一步优化研究提供了平台。
The methanation of CO2via the Sabatier process is gaining interest for power-to-gas (P2G) application. In this work, CO2methanation activity and stability were investigated over Ni/GDC (gadolinium-doped-ceria) catalysts at atmospheric pressure varying reaction temperature (TSET= 300–600 °C) and space velocity (GHSV = 10,000–50,000 h−1). Powder catalysts with different Ni content (15–50 wt.%) were synthesized by the solution combustion synthesis (SCS). The same method was adopted toin situdeposit the Ni/GDC (50 wt.%Ni) coating layer on the cordierite monolith (500 cpsi). The catalysts were characterized by N2adsorption-desorption, X-ray diffraction (XRD), H2temperature programmed reduction (H2-TPR), CO2temperature programmed desorption (CO2-TPD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and scanning electron microscopy (SEM). Temperature profiles along the structured catalytic bed were discussed to interpret the experimental results.Catalytic performance increased by increasing the Ni content due to enhanced metal-to-support interaction, basicity and oxygen vacancies. Uniform, thin and high-resistance catalytic layers werein situdeposited on the cordierite monoliths by the fully reproducible SCS method. Structured catalysts showed high methane productivity per unit weight of catalyst due to simultaneous low catalytic loading and high flow rate. Excellent stability was observed over 200 h of time-on-stream. The results reported in this manuscript pinpointed on the important aspects of realizing CO2methanation on structured catalysts, providing a platform for further optimization studies.