当前位置: X-MOL 学术Appl. Catal. B Environ. Energy › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Highly selective and stable nickel catalysts supported on ceria promoted with Sm2O3, Pr2O3 and MgO for the CO2 methanation
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-09-21 , DOI: 10.1016/j.apcatb.2020.119562
G.I. Siakavelas , N.D. Charisiou , S. AlKhoori , A.A. AlKhoori , V. Sebastian , S.J. Hinder , M.A. Baker , I.V. Yentekakis , K. Polychronopoulou , M.A. Goula

The present work reports on the investigation of the catalytic performance for the methanation of CO2 over Ni catalysts based on CeO2, and for the first time, of Ni catalysts based on binary CeO2-based oxides Sm2O3-CeO2, Pr2O3-CeO2 and MgO-CeO2. The supports were obtained using the microwave assisted sol-gel method under reflux, while the catalysts were prepared by the wet impregnation method. For the investigation of the morphological, textural, structural and other intrinsic properties of the catalytic materials a variety of characterization techniques were used, i.e., Raman spectroscopy, XRD, N2 physisorption-desorption, CO2-TPD, H2-TPR, H2-TPD, XPS and TEM. Carbon deposition and sintering were investigated using TEM. It was shown that the addition of Sm3+ or Pr3+, incorporated into the lattice of CeO2, generated oxygen vacancies, but the Ni/Pr-Ce catalyst was found to possess more surface oxygen vacancies (e.g. Ce4+-Ov-Pr3+ entities). Moreover, modification of CeO2 using Sm3+ or Pr3+ restricted the agglomeration of nickel active sites and led to the genesis of Lewis basic positions. These characteristics improved the hydrogenation reaction at lower temperature. On the other hand, the addition of Mg2+ resulted at strong metal support interactions reinforcing the resistance of the Ni/Mg-Ce catalyst against sintering. Moreover, the addition of Sm3+, Pr3+ and Mg2+ cations increased the overall basicity and the moderate adsorption sites and led to the formation of smaller Ni nano particles; these physico-chemical properties enhanced the CO2 methanation reaction. Finally, the activity experiments (WGHSV = 25,000 mL g−1 h−1, H2/CO2 = 4:1, T =350 °C) showed that at lower reaction temperature the Ni/Pr-Ce had the highest catalytic performance in terms of CO2 conversion (54.5%) and CH4 yield (54.5%) and selectivity (100%). The TOF values were found to follow the order Ni/Pr-Ce >> Ni/Mg-Ce > Ni/Sm-Ce > Ni/Ce.



中文翻译:

Sm 2 O 3,Pr 2 O 3和MgO促进CO 2甲烷化负载在二氧化铈上的高选择性和稳定镍催化剂。

本工作报告了关于研究基于CeO 2的Ni催化剂上CO 2甲烷化甲烷化性能的研究,并且首次报道了基于二元CeO 2基氧化物Sm 2 O 3 -CeO 2的Ni催化剂的甲烷化性能, Pr 2 O 3 -CeO 2和MgO-CeO 2。使用微波辅助溶胶-凝胶法在回流下获得载体,同时通过湿浸渍法制备催化剂。为了研究催化材料的形态,结构,结构和其他固有特性,使用了多种表征技术,即拉曼光谱法,XRD,N 2物理吸附-解吸,CO 2 -TPD,H 2 -TPR,H 2 -TPD,XPS和TEM。使用TEM研究了碳沉积和烧结。结果表明,在CeO 2晶格中加入Sm 3+或Pr 3+会产生氧空位,但发现Ni / Pr-Ce催化剂具有更多的氧空位。表面氧空位(例如Ce 4+ -Ov-Pr 3+实体)。此外,使用Sm 3+或Pr 3+修饰CeO 2限制了镍活性位的团聚,并导致了Lewis基本位置的产生。这些特性改善了在较低温度下的氢化反应。另一方面,Mg 2+的添加导致较强的金属载体相互作用,从而增强了Ni / Mg-Ce催化剂的抗烧结性。此外,添加了Sm 3+,Pr 3+和Mg 2+阳离子增加了整体碱度和中等的吸附位,并导致形成了较小的Ni纳米颗粒。这些物理化学性质增强了CO 2甲烷化反应。最后,活性实验(WGHSV = 25,000 mL g -1  h -1,H 2 / CO 2  = 4:1,T = 350°C)表明,在较低的反应温度下,Ni / Pr-Ce具有最高的催化性能在CO 2转化率(54.5%)和CH 4产率(54.5%)和选择性(100%)方面。发现TOF值遵循以下顺序:Ni / Pr-Ce >> Ni / Mg-Ce> Ni / Sm-Ce> Ni / Ce。

更新日期:2020-09-30
down
wechat
bug