Size Effect of Surface Defects Dictates Reactivity for Nitrogen Electrofixation

Yuntong Sun, Gonggong Lu, Zhiqi Wang, Xuheng Li, Yinghao Li, Nicole L.D. Sui, Wenjun Fan, Ao Wang, Bo Yuan, Junjie Wang, Jong Min Lee

Research output: Contribution to journalArticlepeer-review

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 languageEnglish
Article numbere202425112
JournalAngewandte Chemie - International Edition
Volume64
Issue number19
DOIs
StatePublished - 5 May 2025

Keywords

  • Ammonia production
  • Defect engineering
  • Electrocatalysis
  • Nitrogen reduction reaction
  • Size effect

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