<p>Coupling N<sub>2</sub> electroreduction with kinetically and/or thermodynamically favored oxidation reactions in one system can realize the co-production of NH<sub>3</sub> and value-added oxygen-containing fine chemicals at lower energy consumption. Here, a new N<sub>2</sub> electrolysis system based on nitrogen-doped carbon-supported Bi<sub>2</sub>O<sub>3</sub> and NiO catalysts (Bi<sub>2</sub>O<sub>3</sub>/NC and NiO/NC) is demonstrated, in which the methanol oxidation reaction in the anode to make formic acid is coupled with N<sub>2</sub> electroreduction for NH<sub>3</sub>. The optimal NH<sub>3</sub> yield of <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\(2.79 \, \mu{\rm g}_{{\rm NH}_3} \, {\rm h}^{-1} \, {\rm cm}^{-2}\)</EquationSource> <EquationSource Format="MATHML"><math display="block"> <mn>2.79</mn> <mspace width="thinmathspace" /> <mi>μ</mi> <msub> <mrow> <mi mathvariant="normal">g</mi> </mrow> <mrow> <msub> <mrow> <mi mathvariant="normal">N</mi> <mi mathvariant="normal">H</mi> </mrow> <mn>3</mn> </msub> </mrow> </msub> <mspace width="thinmathspace" /> <msup> <mrow> <mi mathvariant="normal">h</mi> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> <mspace width="thinmathspace" /> <msup> <mrow> <mi mathvariant="normal">cm</mi> </mrow> <mrow> <mo>−</mo> <mn>2</mn> </mrow> </msup> </math></EquationSource> </InlineEquation> is achieved at the voltage of 2.35 V with a high Faradaic efficiency of 5.04%, surpassing the state-of-the-art reported N<sub>2</sub> reduction-methanol oxidation coupling electrocatalysis system. This study highlights the critical role of anode coupling strategy in enabling efficient electrochemical NH<sub>3</sub> synthesis.</p>

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Co-electrosynthesis of ammonia and formic acid over nitrogen-doped carbon-supported Bi2O3 and NiO catalysts

  • Wei Zhang,
  • Yu Zhao,
  • Zhengnan Ju,
  • Ying Sun,
  • Ruoxing Li,
  • Kaiqi Yu,
  • Yunke Fang,
  • Zhiyuan Yang,
  • Shuyao Wu,
  • Hui Li,
  • Yang Fu,
  • Hua Fan,
  • Jieshan Qiu,
  • Chang Yu,
  • Jingang Wang,
  • Tianyi Ma

摘要

Coupling N2 electroreduction with kinetically and/or thermodynamically favored oxidation reactions in one system can realize the co-production of NH3 and value-added oxygen-containing fine chemicals at lower energy consumption. Here, a new N2 electrolysis system based on nitrogen-doped carbon-supported Bi2O3 and NiO catalysts (Bi2O3/NC and NiO/NC) is demonstrated, in which the methanol oxidation reaction in the anode to make formic acid is coupled with N2 electroreduction for NH3. The optimal NH3 yield of \(2.79 \, \mu{\rm g}_{{\rm NH}_3} \, {\rm h}^{-1} \, {\rm cm}^{-2}\) 2.79 μ g N H 3 h 1 cm 2 is achieved at the voltage of 2.35 V with a high Faradaic efficiency of 5.04%, surpassing the state-of-the-art reported N2 reduction-methanol oxidation coupling electrocatalysis system. This study highlights the critical role of anode coupling strategy in enabling efficient electrochemical NH3 synthesis.