Urea electrolysis is ap rospective technology for simultaneous H 2 production and nitrogen suppression in the process of water being used for energy production. Its sustainability is currently founded on innocuous N 2 products; however,w ed iscovered that prevalent nickel-based catalysts could generally over-oxidizeu rea into NO 2 À products with % 80 %F aradaic efficiencies,p osing potential secondary hazards to the environment. Trace amounts of over-oxidized NO 3À and N 2 Owere also detected. Using 15 Nisotopes and urea analogues,w ed erived an itrogen-fate network involving aN O 2 À -formation pathwayv ia OH À -assisted C À Nc leavage and two N 2 -formation pathwaysv ia intra-and intermolecular coupling.D FT calculations confirmed that C À Nc leavage is energetically more favorable.I nspired by the mechanism, ap olyaniline-coating strategy was developed to locally enrich urea for increasing N 2 production by af actor of two.T hese findings provide complementary insights into the nitrogen fate in water-energy nexus systems.
Over‐oxidation in alkaline urea oxidation to dominate NO2− formation over N2 has been discovered by Xuejing Yang, Yefei Li, Ming Gong, and co‐workers in their Research Article on page 26656. The identified nitrogen conversion network and reaction mechanism has important implications for sustainable chemistry and inspires new rationales for novel catalyst designs for the electrochemical urea oxidation into N2 products.
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