Citation: Chengcheng Zhao, Yonghui Zhao, Shenggang Li, Yuhan Sun. Effect of Pd doping on CH₄ reactivity over Co₃O₄ catalysts from density-functional theory calculations[J]. Chinese Journal of Catalysis, ;2017, 38(5): 813-820. doi: 10.1016/S1872-2067(17)62817-1 shu

Effect of Pd doping on CH₄ reactivity over Co₃O₄ catalysts from density-functional theory calculations

Chengcheng Zhao ^a,b,c, ,
Yonghui Zhao ^a ,
Shenggang Li ^a,c ,
Yuhan Sun ^a,c

a. CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China;
b. University of Chinese Academy of Sciences, Beijing 100049, China;
c. School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China

Received Date: 27 January 2017
Revised Date: 24 February 2017

Fund Project: This work was supported by the National Natural Science Foundation of China (21473233, 21403277) and the Energy Technologies Institute LLP, UK.

Palladium oxide (PdO_x) and cobalt oxide (Co₃O₄) are efficient catalysts for methane (CH₄) combustion, and Pd-doped Co₃O₄ catalysts have been found to exhibit better catalytic activities, which suggest synergism between the two components. We carried out first-principles calculations at the PBE+U level to investigate the Pd-doping effect on CH₄ reactivity over the Co₃O₄ catalyst. Because of the structural complexity of the Pd-doped Co₃O₄ catalyst, we built Pd-doped catalyst models using Co₃O₄(001) slabs with two different terminations and examined CH₄ reactivity over the possible Pd-O active sites. A low energy barrier of 0.68 eV was predicted for CH₄ dissociation over the more reactive Pd-doped Co₃O₄(001) surface, which was much lower than the 0.98 and 0.89 eV that was predicted previously over the more reactive pure Co₃O₄(001) and (011) surfaces, respectively. Using a simple model, we predicted CH₄ reaction rates over the pure Co₃O₄(001) and (011) surfaces, and Co₃O₄(001) surfaces with different amounts of Pd dopant. Our theoretical results agree well with the available experimental data, which suggests a strong synergy between the Pd dopant and the Co₃O₄ catalyst, and leads to a significant increase in CH₄ reaction rate.
- Spinel cobalt oxide,
- Palladium dopant,
- Methane combustion,
- Density function theory calculation,
- Reaction rate,
- Collision theory
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Effect of Pd doping on CH₄ reactivity over Co₃O₄ catalysts from density-functional theory calculations