Abstract

Graphene is extremely promising for next-generation spintronics applications; however, realizing graphene-based room-temperature magnets remains a great challenge. Here, we demonstrate that robust room-temperature ferromagnetism with TC up to ∼400 K and saturation magnetization of 0.11 emu g−1 (300 K) can be achieved in graphene by embedding isolated Co atoms with the aid of coordinated N atoms. Extensive structural characterizations show that square-planar Co-N4 moieties were formed in the graphene lattices, where atomically dispersed Co atoms provide local magnetic moments. Detailed electronic structure calculations reveal that the hybridization between the d electrons of Co atoms and delocalized pz electrons of N/C atoms enhances the conduction-electron mediated long-range magnetic coupling. This work provides an effective means to induce room-temperature ferromagnetism in graphene and may open possibilities for developing graphene-based spintronics devices.

Highlights

  • Graphene is extremely promising for next-generation spintronics applications; realizing graphene-based room-temperature magnets remains a great challenge

  • Co K-edge Xray absorption near edge structure (XANES) spectra (Fig. 1f and Supplementary Fig. 3), Fourier-transformed (FT) k3-weighted Co K-edge extended X-ray absorption fine structure (EXAFS) spectra (Fig. 1g), and wavelet transform (WT) analysis (Fig. 1h) show that Co exists as isolated atoms in graphene

  • In summary, we have explored the possibility of achieving stable room-temperature ferromagnetic ordering in graphene by embedding single magnetic transition metal (TM) atoms in the lattice via the strong chemical bonds in the TM-Nx moieties

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Summary

Introduction

Graphene is extremely promising for next-generation spintronics applications; realizing graphene-based room-temperature magnets remains a great challenge. Motivated by the above consideration, we propose a coordination atom assisted strategy by embedding magnetic TM into graphene lattices under the assistance of coordinated N atoms, where stable room-temperature ferromagnetism can be achieved in graphene This strategy is exemplified by the singlemetal-atomic Co-N4 moiety doped graphene, which was synthesized via an impregnation-pyrolysis method, and exhibits unprecedented ferromagnetic orderings with Curie temperature (TC) up to ∼400 K. The Co-N4 doped graphene possesses unique electronic structure where only one spin channel crosses the Fermi level, which is beneficial for the generation of spin-polarized current in spintronics[31] This deliberately designed strategy opens up an avenue for the development of graphene-based spintronic devices

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