Ni/CeO2 Nanocatalysts with Optimized CeO2 Support Morphologies for CH4 Oxidation

被引:26
作者
Chen, Junjie [1 ]
Pham, Hien N. [2 ,3 ]
Mon, Tala [1 ]
Toops, Todd J. [4 ]
Datye, Abhaya K. [2 ,3 ]
Li, Zhenglong [5 ]
Kyriakidou, Eleni A. [1 ]
机构
[1] Univ Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
[2] Univ New Mexico, Dept Chem & Biol Engn, Albuquerque, NM 87131 USA
[3] Univ New Mexico, Ctr Microengn Mat, Albuquerque, NM 87131 USA
[4] Oak Ridge Natl Lab, Energy & Transportat Sci Div, Oak Ridge, TN 37831 USA
[5] Oak Ridge Natl Lab, Mfg Sci Div, Oak Ridge, TN 37831 USA
关键词
Ni; CeO2; methane oxidation; morphology control; redox properties; support effect; METHANE COMBUSTION; CERIA CATALYSTS; ACTIVE-SITES; PROPANE; OXYGEN; DEHYDROGENATION; NANOCRYSTALS; SENSITIVITY;
D O I
10.1021/acsanm.2c05496
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Catalytic oxidation of CH4 over nonprecious Ni/CeO2 catalysts has attracted wide attention. Controlling the morphology of a CeO2 support can enhance the CH4 oxidation activity without changing the catalyst composition. Herein, a series of 2 wt % Ni/CeO2 nanocatalysts with different CeO2 support morphologies (nanoparticles (P), rods (R), cubes (C)) and synthetic procedures (precipitation, sol-gel (SG)) were evaluated for their CH4 oxidation performance. The redox properties of CeO2 supports and corresponding Ni loaded catalysts were characterized by H2-temperature-programmed reduction and oxygen storage capacity (OSC) measurements. The relationship among the CeO2 morphologies, surface areas, redox properties, and CH4 oxidation activity for both CeO2 supports and Ni/CeO2 catalysts was established. The findings suggest that CeO2-R has a greater amount of surface oxygen vacancies as well as an improved OSC and CH4 oxidation activity compared to CeO2-P and CeO2-C supports. The same CH4 oxidation activity pattern was observed for the Ni containing catalysts (Ni/CeO2-R > Ni/CeO2-P > Ni/CeO2-C). Increasing the CeO2 surface area by using a solgel synthesis method (CeO2-SG) improved the amount of surface oxygen vacancies and CH4 oxidation performance of CeO2-SG and Ni/CeO2-SG compared to CeO2-R and Ni/CeO2-R, respectively. Finally, all studied Ni/CeO2 nanocatalysts showed improved hydrothermal stability compared to conventional Pd/Al2O3.
引用
收藏
页码:4544 / 4553
页数:10
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