Renewable-compatible urea electrosynthesis enabled by dynamic asymmetric catalytic domains

Electrocatalytic C–N coupling offers a sustainable route to produce urea from CO2 and nitrate, yet most catalysts operate within narrow potential windows, limiting their performance under fluctuating renewable power. Here we show that dynamic asymmetric catalytic domains composed of Cu single-atoms (CuSA) and Cu-Rh single-atom alloys (Cu1RhSAA), in which asymmetric sites are bridged by an elastic Cu/Rh–O–V electronic bridge. These two Cu environments promote initial C–N coupling and subsequent hydrogenation, respectively, while the elastic electronic bridges redistribute excess charge and help preserve the local coordination environment as the potential changes. This design achieves a urea Faradaic efficiency (FE) > 65% from −0.2 to −0.6 V and reaches a yield rate of 234.39 mmol h−1 g−1. Under a seven-day variable-potential protocol informed by solar irradiance, the mean urea FE is 70.0 ± 8.0%. Techno-economic and life-cycle assessments indicate favorable environmental and economic potential. These results establish dynamic asymmetric catalytic domains as a general strategy for scalable, renewable-compatible electrosynthesis of nitrogen-containing products. Fluctuating renewable electricity challenges selective urea electrosynthesis because catalysts often operate within narrow potential windows. Here, the authors design dynamic asymmetric copper–rhodium catalytic domains that buffer charge and sustain urea production under variable electrical input.