Scholarlink

<p>Nitrite (NO<sub>2</sub><sup>⁻</sup>) is a high-value chemical pivotal to agriculture and pharmaceuticals, yet its conventional via the Ostwald process is energy-intensive and polluting. Electrochemical urea oxidation reaction (UOR) offers a sustainable NO<sub>2</sub><sup>⁻</sup> synthesis pathway with concurrent energy-saving hydrogen (H<sub>2</sub>) production, but suffers from non-selective N<sub>2</sub>/CO<sub>2</sub> pathways. Here, we report Cr<sup>3+</sup> Lewis acid sites in Ni<sub>3</sub>S<sub>2</sub> that act as hydroxyl (OH<sup>⁻</sup>) pumps, dynamically spilling OH<sup>⁻</sup> to adjacent Ni sites via a Lewis acid-base interaction. This triggers a urea-to-NO<sub>2</sub><sup>⁻</sup> pathway, achieving a NO<sub>2</sub><sup>⁻</sup> yield of 120.98 mg h<sup>-1</sup> cm<sup>-2</sup> (600 mA cm<sup>-2</sup>). The OH<sup>⁻</sup> spillover accelerates C-N cleavage while suppressing N-N coupling, enabling energy-saving H<sub>2</sub> production (3.7 kWh m<sup>-3</sup> at 500 mA cm<sup>-2</sup>) and Zn-urea-air batteries (charging potential 288 mV lower than Zn-air). Techno-economic analysis reveals $1,210.5 per ton of urea processed at 400 mA cm<sup>-2</sup>. This work establishes OH<sup>⁻</sup> spillover as a universal design principle for selective electrocatalysis.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Lewis acid-triggered hydroxyl spillover enables selective urea electrooxidation to nitrite with concurrent energy-saving hydrogen production

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年1月13日

查看全文
  • Chao Fan,
  • Meng Zhang,
  • Yunchao Li,
  • Yali Zhang,
  • Yan-Qin Wang,
  • Feilong Gong,
  • Jian Liu

摘要

Nitrite (NO2⁻) is a high-value chemical pivotal to agriculture and pharmaceuticals, yet its conventional via the Ostwald process is energy-intensive and polluting. Electrochemical urea oxidation reaction (UOR) offers a sustainable NO2⁻ synthesis pathway with concurrent energy-saving hydrogen (H2) production, but suffers from non-selective N2/CO2 pathways. Here, we report Cr3+ Lewis acid sites in Ni3S2 that act as hydroxyl (OH⁻) pumps, dynamically spilling OH⁻ to adjacent Ni sites via a Lewis acid-base interaction. This triggers a urea-to-NO2⁻ pathway, achieving a NO2⁻ yield of 120.98 mg h-1 cm-2 (600 mA cm-2). The OH⁻ spillover accelerates C-N cleavage while suppressing N-N coupling, enabling energy-saving H2 production (3.7 kWh m-3 at 500 mA cm-2) and Zn-urea-air batteries (charging potential 288 mV lower than Zn-air). Techno-economic analysis reveals $1,210.5 per ton of urea processed at 400 mA cm-2. This work establishes OH⁻ spillover as a universal design principle for selective electrocatalysis.