<p>The electrocatalytic conversion of nitrate (NO<sub>3</sub><sup>−</sup>) in NO<sub>3</sub><sup>−</sup>-rich wastewater streams to ammonia (NH<sub>3</sub>) can promote reactive nitrogen recovery and decentralized energy storage. However, it remains challenging to efficiently produce NH<sub>3</sub> from NO<sub>3</sub><sup>−</sup>. Here we designed a high-performance CuPd bimetallic catalyst with abundant Cu–Pd hydride interfaces under electrochemical NO<sub>3</sub><sup>−</sup> reduction reaction conditions. The NH<sub>3</sub> production rate in a membrane electrode assembly electrolyser reached ∼19.9 mmol h<sup>−1</sup> cm<sup>−2</sup> with a current density of 5.0 A cm<sup>−2</sup> at ∼2.56 V, and the catalyst remained stable at 2.0 A cm<sup>−2</sup> with an NH<sub>3</sub> Faradaic efficiency of ∼86.8% for 1,000 h. Mechanistic studies attribute the high performance to the Cu–Pd hydride interface structure that facilitates *NO hydrogenation and *NH<sub>3</sub> desorption. Furthermore, we successfully extended the high performance to an electrolyser stack with five 100-cm<sup>2</sup> membrane electrode assemblies. The demonstrated scalability and long-term robustness underscore the industrial applicability of this approach for upstream integration with NO<sub><i>x</i></sub> sources.</p><p></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

Copper–palladium hydride interfaces promote electrochemical ammonia synthesis

  • Yunfan Fu,
  • Shuo Wang,
  • Pengfei Wei,
  • Yi Wang,
  • Rongtan Li,
  • Jiaqi Shao,
  • Dunfeng Gao,
  • Qiang Fu,
  • Guoxiong Wang,
  • Xinhe Bao

摘要

The electrocatalytic conversion of nitrate (NO3) in NO3-rich wastewater streams to ammonia (NH3) can promote reactive nitrogen recovery and decentralized energy storage. However, it remains challenging to efficiently produce NH3 from NO3. Here we designed a high-performance CuPd bimetallic catalyst with abundant Cu–Pd hydride interfaces under electrochemical NO3 reduction reaction conditions. The NH3 production rate in a membrane electrode assembly electrolyser reached ∼19.9 mmol h−1 cm−2 with a current density of 5.0 A cm−2 at ∼2.56 V, and the catalyst remained stable at 2.0 A cm−2 with an NH3 Faradaic efficiency of ∼86.8% for 1,000 h. Mechanistic studies attribute the high performance to the Cu–Pd hydride interface structure that facilitates *NO hydrogenation and *NH3 desorption. Furthermore, we successfully extended the high performance to an electrolyser stack with five 100-cm2 membrane electrode assemblies. The demonstrated scalability and long-term robustness underscore the industrial applicability of this approach for upstream integration with NOx sources.