Ambient ammonia synthesis via palladium-catalyzed electrohydrogenation of dinitrogen at low overpotential
Overpotential
Electrosynthesis
Ammonia production
Reversible hydrogen electrode
DOI:
10.1038/s41467-018-04213-9
Publication Date:
2018-04-30T09:59:07Z
AUTHORS (6)
ABSTRACT
Electrochemical reduction of N2 to NH3 provides an alternative the Haber-Bosch process for sustainable, distributed production when powered by renewable electricity. However, development such has been impeded lack efficient electrocatalysts reduction. Here we report electroreduction on palladium nanoparticles in phosphate buffer solution under ambient conditions, which exhibits high activity and selectivity with yield rate ~4.5 μg mg-1Pd h-1 a Faradaic efficiency 8.2% at 0.1 V vs. reversible hydrogen electrode (corresponding low overpotential 56 mV), outperforming other catalysts including gold platinum. Density functional theory calculations suggest that unique originates from its balanced evolution Grotthuss-like hydride transfer mechanism α-palladium lowers free energy barrier hydrogenation *N2H, rate-limiting step electrosynthesis.
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