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author:

Wang, Jingnan (Wang, Jingnan.) [1] | Zhao, Kaiheng (Zhao, Kaiheng.) [2] | Yao, Yongbin (Yao, Yongbin.) [3] | Xue, Fan (Xue, Fan.) [4] | Lu, Fei (Lu, Fei.) [5] | Yan, Wensheng (Yan, Wensheng.) [6] | Yuan, Fangli (Yuan, Fangli.) [7] | Wang, Xi (Wang, Xi.) [8]

Indexed by:

Scopus SCIE

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 mg(cat)(-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 similar to 21.8% and similar to 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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Community:

  • [ 1 ] [Wang, Jingnan]Fuzhou Univ, Inst Mol Engn Plus, Coll Chem, Fuzhou 350108, Peoples R China
  • [ 2 ] [Wang, Jingnan]China Univ Petr, State Key Lab Heavy Oil Proc, Beijing, Peoples R China
  • [ 3 ] [Zhao, Kaiheng]Chinese Acad Sci, Key Lab Photochem, Inst Chem, Beijing 100190, Peoples R China
  • [ 4 ] [Yao, Yongbin]Beijing Jiaotong Univ, Sch Phys Sci & Engn, Key Lab Luminescence & Opt Informat, Minist Educ, Beijing 100044, Peoples R China
  • [ 5 ] [Xue, Fan]Beijing Jiaotong Univ, Sch Phys Sci & Engn, Key Lab Luminescence & Opt Informat, Minist Educ, Beijing 100044, Peoples R China
  • [ 6 ] [Wang, Xi]Beijing Jiaotong Univ, Sch Phys Sci & Engn, Key Lab Luminescence & Opt Informat, Minist Educ, Beijing 100044, Peoples R China
  • [ 7 ] [Lu, Fei]Yangzhou Univ, Coll Phys Sci & Technol, Yangzhou 225002, Peoples R China
  • [ 8 ] [Yan, Wensheng]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230026, Anhui, Peoples R China
  • [ 9 ] [Yuan, Fangli]Chinese Acad Sci, Inst Proc Engn, State Key Lab Mesosci & Engn, Beijing 100190, Peoples R China

Reprint 's Address:

  • [Wang, Xi]Beijing Jiaotong Univ, Sch Phys Sci & Engn, Key Lab Luminescence & Opt Informat, Minist Educ, Beijing 100044, Peoples R China

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Source :

NATURE COMMUNICATIONS

Year: 2025

Issue: 1

Volume: 16

1 4 . 7 0 0

JCR@2023

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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