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Catalytic methane activation over La1−xSrxScO3−α proton-conducting oxide surface: A comprehensive study
Journal of Catalysis ( IF 6.5 ) Pub Date : 2020-12-23 , DOI: 10.1016/j.jcat.2020.12.011
Dmitriy M. Zakharov , Nikolay A. Zhuravlev , Tatiana A. Denisova , Alexander S. Belozerov , Anna Yu. Stroeva , Emma G. Vovkotrub , Andrei S. Farlenkov , Maxim V. Ananyev

The detailed investigation of the influence of strontium on the methane activation over the state-of-the-art proton-conducting oxide catalyst La1−xSrxScO3−α was carried out using a combination of the novel H/D isotopic exchange method, Raman Spectroscopy, 1H NMR and DFT studies in the temperature range 673 – 973 K, at 10 mbar of CH4 + H2 (95%+5%) mixture. It was found that methane activation occurs via the four parallel channels of the hydrogen adsorption and incorporation mechanism, followed by the formation of methane intermediates with different hydrogen content (CHx species). The dominant type of adsorbed intermediate is governed by the temperature and the surface defect structure, which is in close correlation with the strontium content. The increase of strontium content in La1−xSrxScO3−α drastically increases the catalytic activity due to the surface modification with oxygen deficiencies in the ScO6 octahedron, and stabilisation of the CHx species with a low amount of hydrogen.



中文翻译:

La 1-x Sr x ScO3 质子传导性氧化物表面上的甲烷催化活化作用:综合研究

使用新型的H / D同位素交换技术,对锶对甲烷活化的影响进行了详细研究,研究了最新技术的质子传导氧化物催化剂La 1-x Sr x ScO3 方法,拉曼光谱法,1 H NMR和DFT研究在673 – 973 K的温度范围内,在10 mbar的CH 4  + H 2(95%+ 5%)混合物中。发现甲烷的活化通过氢吸附和结合机理的四个平行通道发生,然后形成具有不同氢含量(CH x种类)。吸附中间体的主要类型受温度和表面缺陷结构的控制,该结构与锶含量密切相关。La 1-x Sr x ScO3 中锶含量的增加由于ScO 6八面体中氧缺陷引起的表面改性以及低氢含量的CH x物种的稳定化而大大提高了催化活性。

更新日期:2021-01-12
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