Ferromagnetic Fe-TiO2 spin catalysts for enhanced ammonia electrosynthesis

Abstract Magnetic field effects (MFE) of ferromagnetic spin electrocatalysts have attracted significant attention due to their potential to enhance catalytic activity under an external magnetic field. However, no ferromagnetic spin catalysts have demonstrated MFE in the electrocatalytic reduction of...

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Main Authors: Jingnan Wang, Kaiheng Zhao, Yongbin Yao, Fan Xue, Fei Lu, Wensheng Yan, Fangli Yuan, Xi Wang
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-56566-7
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author Jingnan Wang
Kaiheng Zhao
Yongbin Yao
Fan Xue
Fei Lu
Wensheng Yan
Fangli Yuan
Xi Wang
author_facet Jingnan Wang
Kaiheng Zhao
Yongbin Yao
Fan Xue
Fei Lu
Wensheng Yan
Fangli Yuan
Xi Wang
author_sort Jingnan Wang
collection DOAJ
description Abstract Magnetic field effects (MFE) of ferromagnetic spin electrocatalysts have attracted significant attention due to their potential to enhance catalytic activity under an external magnetic field. However, no ferromagnetic spin catalysts have demonstrated MFE in the electrocatalytic reduction of nitrate for ammonia (NO3RR), a pioneering approach towards NH3 production involving the conversion from diamagnetic NO3 − to paramagnetic NO. Here, we report the ferromagnetic Fe-TiO2 to investigate MFE on NO3RR. Fe-TiO2 possesses a high density of atomically dispersed Fe sites and exhibits an intermediate-spin state, resulting in magnetic ordering through ferromagnetism. Assisted by a magnetic field, Fe-TiO2 achieves a Faradaic efficiency (FE) of up to 97% and an NH3 yield of 24.69 mg mgcat − 1 at −0.5 V versus reversible hydrogen electrode. Compared to conditions without an external magnetic field, the FE and NH3 yield for Fe-TiO2 under an external magnetic field is increased by ~21.8% and ~ 3.1 times, respectively. In-situ characterization and theoretical calculations show that spin polarization enhances the critical step of NO hydrogenation to NOH by optimizing electron transfer pathways between Fe and NO, significantly boosting NO3RR activity.
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institution Kabale University
issn 2041-1723
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publisher Nature Portfolio
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spelling doaj-art-cc697c1a748e4534826585b7ae382c582025-02-02T12:32:50ZengNature PortfolioNature Communications2041-17232025-01-0116111110.1038/s41467-025-56566-7Ferromagnetic Fe-TiO2 spin catalysts for enhanced ammonia electrosynthesisJingnan Wang0Kaiheng Zhao1Yongbin Yao2Fan Xue3Fei Lu4Wensheng Yan5Fangli Yuan6Xi Wang7Institute of Molecular Engineering Plus, College of Chemistry, Fuzhou UniversityKey Laboratory of Photochemistry, Institute of Chemistry, Chinese Academy of SciencesKey Laboratory of Luminescence and Optical Information, Ministry of Education, School of Physical Science and Engineering, Beijing Jiaotong UniversityKey Laboratory of Luminescence and Optical Information, Ministry of Education, School of Physical Science and Engineering, Beijing Jiaotong UniversityCollege of Physical Science and Technology, Yangzhou UniversityNational Synchrotron Radiation Laboratory, University of Science and Technology of ChinaState Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences (CAS)Key Laboratory of Luminescence and Optical Information, Ministry of Education, School of Physical Science and Engineering, Beijing Jiaotong UniversityAbstract Magnetic field effects (MFE) of ferromagnetic spin electrocatalysts have attracted significant attention due to their potential to enhance catalytic activity under an external magnetic field. However, no ferromagnetic spin catalysts have demonstrated MFE in the electrocatalytic reduction of nitrate for ammonia (NO3RR), a pioneering approach towards NH3 production involving the conversion from diamagnetic NO3 − to paramagnetic NO. Here, we report the ferromagnetic Fe-TiO2 to investigate MFE on NO3RR. Fe-TiO2 possesses a high density of atomically dispersed Fe sites and exhibits an intermediate-spin state, resulting in magnetic ordering through ferromagnetism. Assisted by a magnetic field, Fe-TiO2 achieves a Faradaic efficiency (FE) of up to 97% and an NH3 yield of 24.69 mg mgcat − 1 at −0.5 V versus reversible hydrogen electrode. Compared to conditions without an external magnetic field, the FE and NH3 yield for Fe-TiO2 under an external magnetic field is increased by ~21.8% and ~ 3.1 times, respectively. In-situ characterization and theoretical calculations show that spin polarization enhances the critical step of NO hydrogenation to NOH by optimizing electron transfer pathways between Fe and NO, significantly boosting NO3RR activity.https://doi.org/10.1038/s41467-025-56566-7
spellingShingle Jingnan Wang
Kaiheng Zhao
Yongbin Yao
Fan Xue
Fei Lu
Wensheng Yan
Fangli Yuan
Xi Wang
Ferromagnetic Fe-TiO2 spin catalysts for enhanced ammonia electrosynthesis
Nature Communications
title Ferromagnetic Fe-TiO2 spin catalysts for enhanced ammonia electrosynthesis
title_full Ferromagnetic Fe-TiO2 spin catalysts for enhanced ammonia electrosynthesis
title_fullStr Ferromagnetic Fe-TiO2 spin catalysts for enhanced ammonia electrosynthesis
title_full_unstemmed Ferromagnetic Fe-TiO2 spin catalysts for enhanced ammonia electrosynthesis
title_short Ferromagnetic Fe-TiO2 spin catalysts for enhanced ammonia electrosynthesis
title_sort ferromagnetic fe tio2 spin catalysts for enhanced ammonia electrosynthesis
url https://doi.org/10.1038/s41467-025-56566-7
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AT fanxue ferromagneticfetio2spincatalystsforenhancedammoniaelectrosynthesis
AT feilu ferromagneticfetio2spincatalystsforenhancedammoniaelectrosynthesis
AT wenshengyan ferromagneticfetio2spincatalystsforenhancedammoniaelectrosynthesis
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