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Insight into the impact of rare earth metals in modified Ni/MgO on promoting ammonia decomposition to hydrogen

Journal 2024 · IF 6.7 · 发表于 2024 年 6 月 28 日
作者: Zhixian Bao,Dekang Li,Zhiheng Wang,Yuxin Wen,Lijun Jin,Haoquan Hu
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摘要

The lack of detailed functions of different REMs in NH 3 decomposition to H 2 makes the efficient modified catalysts not rationally be designed though many REMs-modified catalysts have been reported. In this work, the 10Ni/A 1 Mg 4 O α (A = La, Ce, and Y) and 10Ni/MgO, in which supports were synthesized by the sol–gel method and Ni was loaded by the wet-impregnate method, were comparatively investigated to reveal the effect of REMs against NH 3 decomposition reaction. The presence of REMs enhanced the activity of 10Ni/A 1 Mg 4 O α and decreased the activation energy as greatly as by half compared to 10Ni/MgO. The produced H 2 in situ has little impact on the activity of 10Ni/A 1 Mg 4 O α , among which Ce has the most excellent H 2 desorption ability. The intrinsic activity of catalysts was improved better by Ce and Y than La and the best Ni particle size is around 6 nm according to TOF, though the Ni particle is the smallest (4.9 nm) in 10Ni/La 1 Mg 4 O α . The surface structure of catalysts was tuned by doping REMs, forming a solid solution and some defects (oxygen vacancies), which enhanced the interaction between active metal and support with obvious electron transfer from support to Ni obtaining a better Ni dispersion and making NiO easier to be reduced. Additionally, the catalysts doped by La or Ce possess more oxygen vacancy due to the changes of La 2 O 2 CO 3 and the valence of Ce, exhibiting stronger basic sites and better N 2 desorption capacity. The study offers a promising strategy for utilizing appropriate or multiple REMs to synthesize effective catalysts effectively for catalyzing NH 3 decomposition in the future.

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