Citation: Linna Cong, Yonghui Zhao, Shenggang Li, Yuhan Sun. Sr-doping effects on La₂O₃ catalyst for oxidative coupling of methane[J]. Chinese Journal of Catalysis, ;2017, 38(5): 899-907. doi: 10.1016/S1872-2067(17)62823-7 shu

Sr-doping effects on La₂O₃ catalyst for oxidative coupling of methane

Linna Cong ^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: 23 February 2017
Revised Date: 23 March 2017

Fund Project: This work was supported by the National Natural Science Foundation of China (21473233, 21403277), the Frontier Science Program of Shell Global Solutions International B.V. (PT32281), the Ministry of Science and Technology of China (2016YFA0202802), and the Shanghai Municipal Science and Technology Commission (14ZR1444600).

Density-functional theory calculations were carried out to study the strontium (Sr)-doping effect on methane activation over a lanthanum-oxide (La₂O₃) catalyst for the oxidative coupling of methane (OCM) using the cluster model. Eight Sr-doped La₂O₃ cluster models were built from pure La₂O₃ clusters that were used previously to model the La₂O₃ catalyst. These form two distinct categories, namely, those without a radical character (LaSrO₂(OH), La₂SrO₄, La₃SrO₅(OH), and La₅SrO₈(OH)) and those with a radical character (LaSrO₃, La₂SrO₄(OH), La₃SrO₆, and La₅SrO₉). The potential-energy surface for CH₄ activation to form a CH₃ radical at different Sr–O and La–O pair sites on these Sr-doped La₂O₃ clusters was calculated to study the Sr-doping effect on the OCM catalytic activity. CH₄ physisorption and chemisorption energies, and activation barriers, and CH₃ desorption energies were predicted. Compared with the pure La₂O₃ clusters, in general, the Sr-doped La₂O₃ clusters are thermodynamically and kinetically more reactive with CH₄. For the Sr-doped La₂O₃ clusters without the radical character, the Sr–O pair site is more reactive with CH₄ than the La–O pair site, although a direct release of the CH₃ radical is also highly endothermic as in the case of the pure La₂O₃ clusters. In contrast, for the Sr-doped La₂O₃ clusters with a radical character, the activation of CH₄ at the oxygen radical site and the release of the CH₃ radical are much easier. Thus, our calculations suggest that the Sr dopant prompts the OCM catalytic activity of the La₂O₃ catalyst by providing a highly active oxygen-radical site and by strengthening the basicity of the M–O pair site, which leads to lower CH₄ activation energies and lower CH₃ desorption energies.
- Methane activation,
- Methyl radical generation,
- Cluster models,
- Density functional theory,
- Strontium doping,
- Lanthanum oxide
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Sr-doping effects on La₂O₃ catalyst for oxidative coupling of methane