Abstract
Electrocatalytic nitrogen reduction reaction (eNRR) offers a sustainable pathway for ammonia (NH3) production. Defect engineering enhances eNRR activity but can concurrently amplify the competing hydrogen evolution reaction (HER), posing challenges for achieving high selectivity. Herein, VOx with systematically tuned defect sizes is engineered to establish a structure–activity relationship between defect size and eNRR performance. In situ spectroscopy and theoretical calculations reveal that medium-sized defects (VOx-MD, 1–2 nm) provide an optimal electronic environment for enhanced N2 adsorption and activation while maintaining spatial flexibility to facilitate efficient hydrogenation. Consequently, VOx-MD exhibits outstanding eNRR performance, achieving an NH3 yield rate of 81.94 ± 1.45 µg h−1 mg−1 and a Faradaic efficiency of 31.97 ± 0.75 % at −0.5 V (vs RHE). These findings highlight the critical role of defect size in governing eNRR activity, offering a scalable strategy for designing advanced catalysts for competitve electrocatalytic reactions.
Original language | English |
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Article number | e202425112 |
Journal | Angewandte Chemie - International Edition |
Volume | 64 |
Issue number | 19 |
DOIs | |
State | Published - 5 May 2025 |
Keywords
- Ammonia production
- Defect engineering
- Electrocatalysis
- Nitrogen reduction reaction
- Size effect