Urea Electrosynthesis from Nitrate and CO2 on Diatomic Alloys

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Abstract
Urea electrosynthesis from co–electrolysis of NO3 − and CO2 (UENC) offers a promising technology for achieving sustainable and efficient urea production. Herein, a diatomic alloy catalyst (CuPd1Rh1–DAA), with mutually isolated Pd and Rh atoms alloyed on Cu substrate, is theoretically designed and experimentally confirmed to be a highly active and selective UENC catalyst. Combining theoretical computations and operando spectroscopic characterizations reveals the synergistic effect of Pd1–Cu and Rh1–Cu active sites to promote the UENC via a tandem catalysis mechanism, where Pd1–Cu site triggers the early C–N coupling and promotes *CO2NO2–to–*CO2NH steps, while Rh1–Cu site facilitates the subsequent protonation step of *CO2NH2 to *COOHNH2 toward the urea formation. Impressively, CuPd1Rh1–DAA assembled in a flow cell presents the highest urea Faradaic efficiency of 72.1% and urea yield rate of 53.2 mmol h−1 gcat−1 at −0.5 V versus RHE, representing nearly the highest performance among all reported UENC catalysts.
Funding Information
  • National Natural Science Foundation of China (52161025, 52174345, 52064032, 22075211)

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