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<p>Plasma-electrolysis tandem systems can facilitate ammonia (NH<sub>3</sub>) production from air and water under ambient conditions via an ‘air → NO<sub><i>x</i></sub> → NO<sub><i>x</i></sub><sup>−</sup> → NH<sub>3</sub>’ pathway. However, NH<sub>3</sub> yields are limited due to a lack of process intensification between plasma generation and electrocatalytic conversion. Here we report a modified cobalt cathode enriched with twin boundaries (TBs) and stacking faults (SFs) (TB/SF-Co) for selective NO<sub>2</sub><sup>−</sup> reduction. Mechanistic analyses reveal that TB/SF defects upshift the Co <i>d</i>-band centre which strengthens NO<sub>2</sub><sup>−</sup> adsorption and promotes hydrogenation of intermediates. The material achieves a Faradaic efficiency of 96.7% for NO<sub>2</sub><sup>−</sup>-to-NH<sub>3</sub> conversion at a partial current density of −1.73 A cm<sup>−2</sup>. Coupling a cobalt cathode enriched with twin boundaries and stacking faults with a microwave plasma module enables efficient air-to-NH<sub>3</sub> synthesis, achieving an air-to-NO<sub>2</sub><sup>−</sup> rate of 0.745 mol h<sup>−1</sup> and NO<sub>2</sub><sup>−</sup>-to-NH<sub>3</sub> rate of 0.619 mol h<sup>−1</sup> with &gt;95% Faradaic efficiency at a total current of more than 101 A in 100 cm<sup>2</sup> parallel electrolyzers, which rivals or exceeds contemporary benchmarks.</p><p></p>

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Ampere-level ammonia synthesis through grain boundary engineering

  • 期刊论文

  • 发表日期：

    2026年3月18日

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  • Wei Liu,
  • Honghui Ou,
  • Yang Lv,
  • Yuxi Ren,
  • Baorong Xu,
  • Wenkai Teng,
  • He Li,
  • Yang Li,
  • Guidong Yang

摘要

Plasma-electrolysis tandem systems can facilitate ammonia (NH3) production from air and water under ambient conditions via an ‘air → NOx → NOx− → NH3’ pathway. However, NH3 yields are limited due to a lack of process intensification between plasma generation and electrocatalytic conversion. Here we report a modified cobalt cathode enriched with twin boundaries (TBs) and stacking faults (SFs) (TB/SF-Co) for selective NO2− reduction. Mechanistic analyses reveal that TB/SF defects upshift the Co d-band centre which strengthens NO2− adsorption and promotes hydrogenation of intermediates. The material achieves a Faradaic efficiency of 96.7% for NO2−-to-NH3 conversion at a partial current density of −1.73 A cm−2. Coupling a cobalt cathode enriched with twin boundaries and stacking faults with a microwave plasma module enables efficient air-to-NH3 synthesis, achieving an air-to-NO2− rate of 0.745 mol h−1 and NO2−-to-NH3 rate of 0.619 mol h−1 with >95% Faradaic efficiency at a total current of more than 101 A in 100 cm2 parallel electrolyzers, which rivals or exceeds contemporary benchmarks.