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<p>Electroreduction of nitrate (NO<sub>3</sub><sup>‒</sup>) to ammonia (NH<sub>3</sub>) is a promising approach for addressing energy challenges. However, the activity is limited by NO<sub>3</sub><sup>‒</sup> mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO<sub>3</sub><sup>‒</sup> from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO<sub>3</sub><sup>‒</sup> concentration decreases, impeding practical applications in the conversion of NO<sub>3</sub><sup>‒</sup>-to-NH<sub>3</sub>. Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO<sub>3</sub><sup>‒</sup> reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS<sub>2</sub> (Ag-MoS<sub>2</sub>) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO<sub>3</sub><sup>‒</sup>. Thus, Ag-MoS<sub>2</sub> exhibits a ~ 28.6-fold NO<sub>3</sub><sup>‒</sup> concentration in the IHP than the counterpart without junction, and achieves near-100% NH<sub>3</sub> Faradaic efficiency with an NH<sub>3</sub> yield rate of ~20 mg h<sup>‒1</sup> cm<sup>‒2</sup> under ultralow NO<sub>3</sub><sup>‒</sup> concentrations.</p>

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Near-Unity Nitrate to Ammonia conversion via reactant enrichment at the solid-liquid interface

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月1日

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  • Wanru Liao,
  • Jun Wang,
  • Yao Tan,
  • Xin Zi,
  • Changxu Liu,
  • Qiyou Wang,
  • Li Zhu,
  • Cheng-Wei Kao,
  • Ting-Shan Chan,
  • Hongmei Li,
  • Yali Zhang,
  • Kang Liu,
  • Chao Cai,
  • Junwei Fu,
  • Beidou Xi,
  • Emiliano Cortés,
  • Liyuan Chai,
  • Min Liu

摘要

Electroreduction of nitrate (NO3‒) to ammonia (NH3) is a promising approach for addressing energy challenges. However, the activity is limited by NO3‒ mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO3‒ from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO3‒ concentration decreases, impeding practical applications in the conversion of NO3‒-to-NH3. Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO3‒ reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS2 (Ag-MoS2) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO3‒. Thus, Ag-MoS2 exhibits a ~ 28.6-fold NO3‒ concentration in the IHP than the counterpart without junction, and achieves near-100% NH3 Faradaic efficiency with an NH3 yield rate of ~20 mg h‒1 cm‒2 under ultralow NO3‒ concentrations.