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<p>Manipulating the selectivity-determining step in the hydrogenation of nitrogen-containing intermediates is critical to achieving high ammonia selectivity in electrocatalytic nitrate reduction. Here, we propose a molecular interface engineering strategy that functionalized with thiol-anchored aromatic ligands to regulate the interfacial binding affinity and activation of key nitrogen-containing intermediates on silver nanocube surfaces. By systematically varying the electronic properties of the substituents, we identify 4-(methylthio)benzaldehyde as the most effective ligand, increasing the ammonia Faradaic efficiency from 50.8% to 98.9% and achieving a yield rate of 14,366.1 μg h<sup>–1</sup> cm<sub>geo</sub><sup>–2</sup> at –0.63 V versus reversible hydrogen electrode. In situ electrochemical characterizations combined with theoretical simulations further reveal that 4-(methylthio)benzaldehyde modification promotes the activation of weakly hydrogen-bonded water molecules and accelerates the hydrogenation of *HNO intermediates. This targeted modulation of interfacial binding affinity offers an effective strategy for selectivity control in electrocatalytic nitrate reduction. The enhanced performance is further validated in a membrane electrode assembly electrolyser, underscoring the practical viability of this molecular design strategy for selective nitrate conversion.</p>

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Aryl sulfur ligand-modulated silver catalysts with tailored binding affinity for selective nitrate-to-ammonia conversion

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月10日

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  • Longcheng Zhang,
  • Yuan Liu,
  • Ling Li,
  • Xiaoning Li,
  • Pengfei Song,
  • Ting Chen,
  • Qian Wu,
  • Justin Zhu Yeow Seow,
  • Kai Tang,
  • Shirong Sun,
  • Xiaodong Guo,
  • Zhichuan J. Xu

摘要

Manipulating the selectivity-determining step in the hydrogenation of nitrogen-containing intermediates is critical to achieving high ammonia selectivity in electrocatalytic nitrate reduction. Here, we propose a molecular interface engineering strategy that functionalized with thiol-anchored aromatic ligands to regulate the interfacial binding affinity and activation of key nitrogen-containing intermediates on silver nanocube surfaces. By systematically varying the electronic properties of the substituents, we identify 4-(methylthio)benzaldehyde as the most effective ligand, increasing the ammonia Faradaic efficiency from 50.8% to 98.9% and achieving a yield rate of 14,366.1 μg h–1 cmgeo–2 at –0.63 V versus reversible hydrogen electrode. In situ electrochemical characterizations combined with theoretical simulations further reveal that 4-(methylthio)benzaldehyde modification promotes the activation of weakly hydrogen-bonded water molecules and accelerates the hydrogenation of *HNO intermediates. This targeted modulation of interfacial binding affinity offers an effective strategy for selectivity control in electrocatalytic nitrate reduction. The enhanced performance is further validated in a membrane electrode assembly electrolyser, underscoring the practical viability of this molecular design strategy for selective nitrate conversion.