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The nitrogen cycle needed for scaled agriculture relies on energy- and carbon-intensive processes and generates nitrate-containing wastewater. Here we focus on an alternative approach—the electrified co-electrolysis of nitrate and CO2 to synthesize urea. When this is applied to industrial wastewater or agricultural runoff, the approach has the potential to enable low-carbon-intensity urea production while simultaneously providing wastewater denitrification. We report a strategy that increases selectivity to urea using a hybrid catalyst: two classes of site independently stabilize the key intermediates needed in urea formation, *CO2NO2 and *COOHNH2, via a relay catalysis mechanism. A Faradaic efficiency of 75% at wastewater-level nitrate concentrations (1,000 ppm NO3− [N]) is achieved on Zn/Cu catalysts. The resultant catalysts show a urea production rate of 16 µmol h−1 cm−2. Life-cycle assessment indicates greenhouse gas emissions of 0.28 kg CO2e per kg urea for the electrochemical route, compared to 1.8 kg CO2e kg−1 for the present-day route.more » « less
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Han, Lili; Cheng, Hao; Liu, Wei; Li, Haoqiang; Ou, Pengfei; Lin, Ruoqian; Wang, Hsiao-Tsu; Pao, Chih-Wen; Head, Ashley R.; Wang, Chia-Hsin; et al (, Nature Materials)
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Nazemi, Mohammadreza; Ou, Pengfei; Alabbady, Abdulaziz; Soule, Luke; Liu, Alan; Song, Jun; Sulchek, Todd A.; Liu, Meilin; El-Sayed, Mostafa A. (, ACS Catalysis)
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