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Highly Effective Ru/BaCeO3 Catalysts on Supports with Strong Basic Sites for Ammonia Synthesis

Journal 2019 · IF 3.698 · 14(16): 2815-2821 · 发表于 2019 年 6 月 11 日
作者: Wei Li,Shuang Wang,Jinping Li
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摘要

Graphical Be well supported ! Two BaCeO 3 supports with strong basic sites were synthesized by a co-precipitation route under different calcination temperatures. BaCeO 3 -a has a high basic density and Ru/BaCeO 3 -a has more oxygen vacancies, which are beneficial for the dissociation of N 2 . Therefore, the 1.25 % Ru/BaCeO 3 -a catalyst exhibits superior performance in ammonia synthesis (see figure). BaCeO 3 -a and BaCeO 3 -b, with strong basic sites, were synthesized by using a co-precipitation method at different calcination temperatures, and used as supports to evaluate their performance in ammonia synthesis. The ammonia synthesis rate with the 1.25 % Ru/BaCeO 3 -a catalyst is 24 mmol g −1 h −1 , which is higher than that of 1.25 % Ru/BaCeO 3 -b catalyst (18 mmol g −1 h −1 ) at 3 MPa and 450 °C. Moreover, the performance of the 4 % Cs-1.25 % Ru/BaCeO 3 -a catalyst was further improved to 28 mmol g −1 h −1 , and no sign of deactivation was observed after a reaction time of 120 h. The XPS and H 2 temperature-programmed reduction analyses indicated that the Ru/BaCeO 3 -a catalyst has more oxygen vacancies than the Ru/BaCeO 3 -b catalyst. In addition, the average Ru particle size of the Ru/BaCeO 3 -a catalyst is closer to 2 nm than the Ru/BaCeO 3 -b catalyst, which promotes the generation of B 5 -type sites (the active site for N 2 dissociation). The CO 2 temperature-programmed desorption analysis indicates that BaCeO 3 -a has a high basic density, which is beneficial for electron transfer to Ru and further facilitates the dissociation of N≡N bonds.

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