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Highly Effective Ru/BaCeO3 Catalysts on Supports with Strong Basic Sites for Ammonia Synthesis
Wei Li1, Shuang Wang2,1, Jinping Li1
1Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, Taiyuan University of Technology, Taiyuan, 030024, P. R. China.
Abstract:
BaCeO3 -a and BaCeO3 -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/BaCeO3 -a catalyst is 24 mmol g-1 h-1 , which is higher than that of 1.25 % Ru/BaCeO3 -b catalyst (18 mmol g-1 h-1 ) at 3 MPa and 450 °C. Moreover, the performance of the 4 % Cs-1.25 % Ru/BaCeO3 -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 H2 temperature-programmed reduction analyses indicated that the Ru/BaCeO3 -a catalyst has more oxygen vacancies than the Ru/BaCeO3 -b catalyst. In addition, the average Ru particle size of the Ru/BaCeO3 -a catalyst is closer to 2 nm than the Ru/BaCeO3 -b catalyst, which promotes the generation of B5 -type sites (the active site for N2 dissociation). The CO2 temperature-programmed desorption analysis indicates that BaCeO3 -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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