Efficient Ammonia Electrosynthesis from Nitrate on Strained Ruthenium Nanoclusters.
By Jie Li, Guangming Zhan, Jianhua Yang, Fengjiao Quan, Chengliang Mao, Yang Liu, Bo Wang, F. Lei, Lejing Li, Alice W M Chan and 8 more. Journal of the American Chemical Society, 2020
797 citations recorded by the source corpus.
The limitations of the Haber-Bosch reaction-particularly high-temperature operation-have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N2 electroreduction is a compelling alternative, but is impeded by a low ammonia production rate (mostly <10 mmol gcat-1 h-1), small partial current density (<1 mA cm-2), and high-selectivity hydrogen-evolving side-reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 mol gcat-1 h-1) than the Haber-Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen-hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm-2 current densities for 100 hours due to the robust subsurface Ru-O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis.
Subfields: Catalysis, Materials Chemistry, Renewable Energy, Sustainability and the Environment
View Paper: https://www.semanticscholar.org/paper/837e0ee9da76e3fef52b63b077ce5e117f1f6a31
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Citations in the corpus
- Efficient conversion of low-concentration nitrate sources into ammonia on a Ru-dispersed Cu nanowire electrocatalyst (2022, positive): “As a result, our Ru-CuNW delivers an industrial-relevant NH 3 production rate of ~ 1 A cm –2 while maintaining a high NH 3 FE of 96% when operating at NO 3– concentrations of typical industrial wastewater (2000 ppm), outperforming previously reported catalysts 31-40 .”