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Efficient Ammonia Electrosynthesis from Nitrate on Strained Ruthenium Nanoclusters.

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.