Harnessing Spin-Lattice Interplay in Metal Nitrides for Efficient Ammonia Electrosynthesis
© 2025 Wiley‐VCH GmbH.
| Publié dans: | Advanced materials (Deerfield Beach, Fla.). - 1998. - (2025) vom: 30. Apr., Seite e2504505 |
|---|---|
| Auteur principal: | |
| Autres auteurs: | , , , , , , |
| Format: | Article en ligne |
| Langue: | English |
| Publié: |
2025
|
| Accès à la collection: | Advanced materials (Deerfield Beach, Fla.) |
| Sujets: | Journal Article ammonia synthesis metal nitrides nitrate reduction paired electro‐refinery system spin polarization manipulation |
| Résumé: | © 2025 Wiley‐VCH GmbH. Metal nitrides, renowned for their spin-lattice-charge interplay, offer vast potential in catalysis, electronics, and energy conversion. However, spin polarization manipulation in these nitrides remains a challenge for multi-electron electrocatalytic processes. This study introduces Co3Mo3N with a low-spin polarization configuration, achieved by incorporating spin-free lattice Mo with 4d orbitals into high-spin polarization Co4N. This innovation delivers outstanding nitrate-to-ammonia electrosynthesis, ranking among the best to date. Mo inclusion induces competing magnetic exchange interactions, reducing the spin polarization degree and enabling rate-determining step of NO2* to NO-OH* conversion via vertex-sharing NMo6 octahedra. A paired electro-refinery with a Co3Mo3N cathode achieves 2 000 mA cm-2 at 2.28 V and sustains an industrial-scale current of 1 000 mA cm-2 for 2,100 h, with an NH3 production rate of ≈70 mg NH3 h-1 cm-2. This work establishes a transformative platform for spin polarization degree-engineered electrocatalysts, driving breakthroughs in energy conversion technologies |
|---|---|
| Description: | Date Revised 30.04.2025 published: Print-Electronic Citation Status Publisher |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202504505 |