Ruthenium-based catalysts supported on carbon xerogels for hydrogen production via ammonia decomposition

催化作用 化学 无机化学 分解 氨生产 碳纤维 材料科学 有机化学 复合数 复合材料
作者
S. Mazzone,T. Goklany,Guangru Zhang,Jinkun Tan,Evangelos I. Papaioannou,F.R. García–García
出处
期刊:Applied Catalysis A-general [Elsevier BV]
卷期号:632: 118484-118484 被引量:39
标识
DOI:10.1016/j.apcata.2022.118484
摘要

Carbon xerogels were synthesised and used as support of ruthenium-based catalysts for the ammonia decomposition reaction. To improve their physical-chemical properties, carbon xerogels were either activated in carbon dioxide atmosphere (for 1 and 5 h), or doped with nitrogen via co-precursor method, using urea as nitrogen source. Un-promoted and sodium-promoted ruthenium catalysts were prepared by incipient wetness impregnation. All catalysts were tested during the ammonia decomposition reaction (1 atm, 100–600 °C), showing high catalytic activity. The 5 h carbon dioxide activation treatment resulted in a decrease in oxygen surface groups (i.e. by 11 wt%) on carbon xerogels surface, and in an increase in the structure crystallinity (i.e. by 15% in the TBurn) of carbon xerogels, resulting in a higher ammonia decomposition reaction rate (i.e. 3.5-fold at 450 °C). Similarly, nitrogen addition to carbon xerogels had a positive effect on the catalysts basicity, enhancing their catalytic performance (i.e. triple reaction rate at 450 °C). The addition of sodium conferred an enhancement in the performance of each catalyst (i.e. reaction rate up to 9 times higher at 450 °C). Two ammonia decomposition reaction runs were performed for all catalysts, to test the performance reproducibility of the catalysts. It was found that un-promoted catalysts exhibited higher reaction rates (i.e. up to 3.5 times at 450 °C) during the second run of reaction due to the larger ruthenium particle size, whereas sodium-promoted catalysts exhibited similar catalytic activity in both reaction runs due to the presence of sodium oxide avoiding the sintering of ruthenium particles.
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