Highly efficient subnanometer Ru-based catalyst for ammonia synthesis via an associative mechanism
[Display omitted] •N-doped carbon supported sub-nano Ru clusters (Ru-SNCs) catalyst was prepared.•Ru-SNCs catalyst showed a higher NH3 synthesis rate than nanoparticle Ru catalyst.•Ru-SNCs catalyst can follow an associative route for NH3 synthesis. The industrial manufacture of ammonia (NH3) using F...
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Veröffentlicht in: | Chinese journal of chemical engineering 2022-03, Vol.43 (3), p.177-184 |
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Sprache: | eng |
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•N-doped carbon supported sub-nano Ru clusters (Ru-SNCs) catalyst was prepared.•Ru-SNCs catalyst showed a higher NH3 synthesis rate than nanoparticle Ru catalyst.•Ru-SNCs catalyst can follow an associative route for NH3 synthesis.
The industrial manufacture of ammonia (NH3) using Fe-based catalyst works under rigorous conditions. For the goal of carbon-neutrality, it is highly desired to develop advanced catalyst for NH3 synthesis at mild conditions to reduce energy consumption and CO2 emissions. However, the main challenge of NH3 synthesis at mild conditions lies in the dissociation of steady NN triple bond. In this work, we report the design of subnanometer Ru clusters (0.8 nm) anchored on the hollow N-doped carbon spheres catalyst (Ru-SNCs), which effectively promotes the NH3 synthesis at mild conditions via an associative route. The NH3 synthesis rate over Ru-SNCs (0.49% (mass) Ru) reaches up to 11.7 mmol NH3·(g cat)−1·h−1 at 400 °C and 3 MPa, which is superior to that of 8.3 mmol NH3·(g cat)−1·h−1 over Ru nanoparticle catalyst (1.20% (mass) Ru). Various characterizations show that the N2H4 species are the main intermediates for NH3 synthesis on Ru-SNCs catalyst. It demonstrates that Ru-SNCs catalyst can follow an associative route for N2 activation, which circumvents the direct dissociation of N2 and results in highly efficient NH3 synthesis at mild conditions. |
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ISSN: | 1004-9541 2210-321X |
DOI: | 10.1016/j.cjche.2022.01.015 |