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<p>The electrocatalytic nitrate reduction reaction (NO<sub>3</sub><sup>-</sup>RR) offers a promising route to sustainable ammonia synthesis, potentially replacing the energy-intensive Haber-Bosch process. While often studied in neutral or alkaline media, NO<sub>3</sub><sup>-</sup>RR in acidic conditions is particularly relevant due to widespread industrial acidic nitrate wastewater, yet it remains challenging due to corrosion and dominant hydrogen evolution. To address this, we designed a corrosion-resistant Ru/WO<sub>3-<i>x</i></sub> heterostructure that spatially separates proton and nitrate adsorption sites. Here, we show that a reverse hydrogen spillover effect, where the WO<sub>3-<i>x</i></sub> support stores and transports protons to surface Ru active sites, dramatically enhances hydrogenation kinetics and suppresses parasitic hydrogen evolution. This catalyst achieves an ammonia Faradaic efficiency of 94.09% at a high current density of 500 mA cm<sup>−2</sup> and a working potential of 0.026 V vs. reversible hydrogen electrode. Furthermore, we demonstrate a sulfide-nitrate “batterolyzer” with a discharge power density of 43.4 mW cm<sup>−2</sup>. This work reveals an effective proton-management strategy for efficient acidic NO<sub>3</sub><sup>-</sup>RR, advancing its potential for coupled ammonia synthesis and wastewater treatment.</p>

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Reverse hydrogen spillover accelerates electrocatalytic nitrate reduction to ammonia on Ru/WO3-x in acidic media

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月16日

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  • Weijie Zhu,
  • Yu-Chang Lin,
  • Jianlong Cong,
  • Mengting Zhao,
  • Jiahao Li,
  • Cong Hao,
  • Jun Jia,
  • Xinlu Wang,
  • Yunhui Huang,
  • Yan-Gu Lin,
  • Gang Yang,
  • Fen Yao,
  • Hanfeng Liang

摘要

The electrocatalytic nitrate reduction reaction (NO3-RR) offers a promising route to sustainable ammonia synthesis, potentially replacing the energy-intensive Haber-Bosch process. While often studied in neutral or alkaline media, NO3-RR in acidic conditions is particularly relevant due to widespread industrial acidic nitrate wastewater, yet it remains challenging due to corrosion and dominant hydrogen evolution. To address this, we designed a corrosion-resistant Ru/WO3-x heterostructure that spatially separates proton and nitrate adsorption sites. Here, we show that a reverse hydrogen spillover effect, where the WO3-x support stores and transports protons to surface Ru active sites, dramatically enhances hydrogenation kinetics and suppresses parasitic hydrogen evolution. This catalyst achieves an ammonia Faradaic efficiency of 94.09% at a high current density of 500 mA cm−2 and a working potential of 0.026 V vs. reversible hydrogen electrode. Furthermore, we demonstrate a sulfide-nitrate “batterolyzer” with a discharge power density of 43.4 mW cm−2. This work reveals an effective proton-management strategy for efficient acidic NO3-RR, advancing its potential for coupled ammonia synthesis and wastewater treatment.