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Researchers developed a novel SnO2/CuOx catalyst for efficient electrocatalytic urea synthesis from CO2 and nitrate. This sustainable nitrogen-carbon route achieves high urea yield and Faradaic efficiency by optimizing C-N coupling.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Electrocatalytic urea synthesis presents a sustainable route for producing valuable chemicals from CO2 and nitrate.
  • Challenges include complex electron transfer and competing side reactions, hindering efficiency.

Purpose of the Study:

  • To design and optimize a heterojunction catalyst for efficient electrocatalytic urea synthesis.
  • To elucidate the reaction mechanism and identify key intermediates.

Main Methods:

  • Fabrication of SnO2/CuOx heterojunction catalysts with controlled Sn:Cu ratios.
  • In situ infrared spectroscopy and operando NMR (1H, 13C, 15N, 17O) for mechanistic studies.
  • Density functional theory (DFT) calculations to investigate reaction pathways and energy barriers.

Main Results:

  • An optimized SnO2/CuOx catalyst (m-SnO2/CuOx, Sn:Cu ratio 1:5.5) selectively promotes N-terminal hydrogenation of nitrate to hydroxylamine (*NH2OH) and C-N coupling with CO.
  • Operando spectroscopy confirmed the formation of urea via a *H2NCHO intermediate.
  • DFT calculations revealed interfacial charge redistribution that lowers energy barriers for urea formation.

Conclusions:

  • Rational design of SnO2/CuOx heterojunctions enables efficient and selective electrocatalytic urea synthesis.
  • Operando characterization and theoretical calculations provide crucial mechanistic insights.
  • The optimized catalyst achieved a urea yield of 215 mmol g-1 h-1 and 72.18% Faradaic efficiency.