Mechanically Alloyed Nd-Fe-B Nanoparticles with Graphitic Carbon Shell: Synthesis, Characterization and Magnetic Properties

Authors

DOI:

https://doi.org/10.65834/jdsi.12.46

Keywords:

Nd-Fe-B nanoparticles, mechanical alloying, graphitic carbon shell encapsulation, chemical vapor deposition, magnetic properties

Abstract

In this study, Nd-Fe-B nanoparticles with permanent magnet properties were synthesized from elemental raw materials using the mechanical alloying (MA) method and subsequently encapsulated with graphitic carbon shell to enhance their thermal and chemical stability for potential electronic applications. Alloy composition Nd ≈ 23.3 wt.%, Fe ≈ 75.7 wt.%, B ≈ 1.0 wt.%, Nd₁₀Fe₈₄B₆ atomic composition, were milled for varying durations 8-10 and 12 h to evaluate the effects of milling duration on magnetic performance. Due to high-energy milling, powder yield remained between 41% and 53%, influenced by particle adhesion and partial melting. X-ray Diffraction (XRD) confirmed the formation of the tetragonal Nd₂Fe₁₄B phase in all MA-synthesized powders, while Dynamic Light Scattering (DLS) and Scanning Electron Microscopy (SEM) analyses verified nanoparticle size and agglomerated morphologies characteristic of welding-fracture-rewelding cycles in MA. Annealing at 900°C for 1 h improved crystallinity and promoted the formation of additional phases, as supported by XRD, SEM and Energy Dispersive Spectroscopy (EDS) results. A Graphitic Carbon Shell (GCS) was successfully deposited on the nanoparticle surfaces via Chemical Vapor Deposition (CVD) under a CH₄/H₂ atmosphere at 950°C; the presence of the carbonaceous coating was confirmed by XRD and elemental mapping. Transmission Electron Microscopy (TEM) analysis revealed the core-shell structure, the number of graphitic carbon shell layers, and the uniformity of the encapsulation surrounding the nanoparticles. Magnetic characterization using Vibrating Sample Magnetometer (VSM) showed variations in coercivity, saturation magnetization and remanence before and after encapsulation. Among all samples, the 10 h milled, annealed and graphitic carbon shell encapsulated sample (NFB2TG) exhibited the most favorable magnetic properties, reaching a coercivity of 185.71 Oe and saturation magnetization of 46.3 emu/g. These results demonstrate that MA followed by annealing and encapsulation GCS is a promising route for producing stable Nd-Fe-B nanoparticles.

References

Ağaoğulları, D., Gökçe, H., Duman, İ., & Öveçoğlu, M. L. (2011). Characterization investigations of ZrB₂/ZrC ceramic powders synthesized by mechanical alloying of elemental Zr, B and C blends. Journal of the European Ceramic Society, 32(7), 1447-1455. https://doi.org/10.1016/j.jeurceramsoc.2011.04.026

Ağaoğulları, D., Madsen, S. J., Öğüt, B., Koh, A. L., & Sinclair, R. (2017). Synthesis and characterization of graphite-encapsulated iron nanoparticles from ball milling-assisted low-pressure chemical vapor deposition. Carbon, 124, 170-179. https://doi.org/10.1016/j.carbon.2017.08.043

Bystrzejewski, M., Lange, H., & Huczko, A. (2007). Carbon encapsulation of magnetic nanoparticles. Fullerenes, Nanotubes and Carbon Nanostructures, 15(3), 167-180. https://doi.org/10.1080/15363830701236357

Chakka, V. M., Altuncevahir, B., Jin, Z. Q., Li, Y., & Liu, J. P. (2006). Magnetic nanoparticles produced by surfactant-assisted ball milling. Journal of Applied Physics, 99(8), Article 08E912. https://doi.org/10.1063/1.2170593

Chen, W., Kim, J., Sun, S., & Chen, S. (2007). Composition effects of FePt alloy nanoparticles on the electro-oxidation of formic acid. Langmuir, 23(22), 11303-11310. https://doi.org/10.1021/la7016648

Coey, J. M. D. (2010). Magnetism and magnetic materials. Cambridge University Press. https://doi.org/10.1017/CBO9780511845000

De Moraes, I. G., Fischbacher, J., Hong, Y., Naud, C., Okuno, H., Masseboeuf, A., Devillers, T., Schrefl, T., & Dempsey, N. M. (2024). Nanofabrication, characterisation and modelling of soft-in-hard FeCo-FePt magnetic nanocomposites. Acta Materialia, 274, Article 119970. https://doi.org/10.1016/j.actamat.2024.119970

Dempsey, N. M. (2009). Hard magnetic materials for MEMS applications. In J. P. Liu, E. Fullerton, O. Gutfleisch, & D. J. Sellmyer (Eds.), Nanoscale magnetic materials and applications (pp. 661-683). Springer. https://doi.org/10.1007/978-0-387-85600-1_22

Goldstein, J. I., Newbury, D. E., Michael, J. R., Ritchie, N. W. M., Scott, J. H. J., & Joy, D. C. (2018). Scanning electron microscopy and X-ray microanalysis (4th ed.). Springer. https://doi.org/10.1007/978-1-4939-6676-9

Gubin, S. P., Spichkin, Y. I., Yurkov, G. Y., & Tishin, A. M. (2002). Nanomaterial for high-density magnetic data storage. Russian Journal of Inorganic Chemistry, 47. https://amtc.ru/publications/articles/5rus.pdf

Hosseinabadi, S., Jafari, M. J., Kokabi, M., & Mohseni, M. (2019). Improving the electromagnetic shielding of fabricated Nd-Fe-B particles by a coating thin carbonaceous layer. Chemical Physics Letters, 739, Article 137015. https://doi.org/10.1016/j.cplett.2019.137015

Iacovacci, V., Lucarini, G., Innocenti, C., Comisso, N., Dario, P., Ricotti, L., & Menciassi, A. (2015). Polydimethylsiloxane films doped with Nd-Fe-B powder: Magnetic characterization and potential applications in biomedical engineering and microrobotics. Biomedical Microdevices, 17(6), Article 112. https://doi.org/10.1007/s10544-015-0024-0

Jia, Z., Li, J., Gao, L., Yang, D., & Kanaev, A. (2023). Dynamic light scattering: A powerful tool for in situ nanoparticle sizing. Colloids and Interfaces, 7(1), Article 15. https://doi.org/10.3390/colloids7010015

Jung, Y., Lee, Y., Yoon, S., & Choi, J. (2024). Synergistic effect of core/shell-structured composite fibers: Efficient recovery of rare-earth elements from spent Nd-Fe-B permanent magnets. Advanced Fiber Materials, 6(6), 1729-1745. https://doi.org/10.1007/s42765-024-00442-4

Lee, S., Jeong, J., Shin, S., Kim, J., Chang, Y., Lee, K., & Kim, J. (2005). Magnetic enhancement of iron oxide nanoparticles encapsulated with poly(d,l-latide-co-glycolide). Colloids and Surfaces A: Physicochemical and Engineering Aspects, 255(1-3), 19-25. https://doi.org/10.1016/j.colsurfa.2004.12.019

Lecerf, I., Angulo-Cervera, J. E., Orlandini-Keller, F., Moritz, P., Mathieu, F., Bourrier, D., Charlot, S., Nicu, L., Leïchlé, T., Devillers, T., Haettel, R., Dempsey, N. M., Blon, T., & Lacroix, L. (2025). A MEMS electromagnetic vibration energy harvester with monolithically integrated Nd-Fe-B micromagnets. Advanced Materials Technologies, 10(10), Article 2401817. https://doi.org/10.1002/admt.202401817

Lim, J., Yeap, S. P., Che, H. X., & Low, S. C. (2013). Characterization of magnetic nanoparticle by dynamic light scattering. Nanoscale Research Letters, 8, Article 381. https://doi.org/10.1186/1556-276X-8-381

Liu, Y. D., Choi, H. J., & Choi, S. (2012). Controllable fabrication of silica encapsulated soft magnetic microspheres with enhanced oxidation-resistance and their rheology under magnetic field. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 403, 133-138. https://doi.org/10.1016/j.colsurfa.2012.04.002

Manaf, A., Al-Khafaji, M., Zhang, P. Z., Davies, H. A., Buckley, R. A., & Rainforth, W. M. (1993). Microstructure analysis of nanocrystalline Fe-Nd-B ribbons with enhanced hard magnetic properties. Journal of Magnetism and Magnetic Materials, 128(3), 307-312. https://doi.org/10.1016/0304-8853(93)90476-I

Mehrifar, Y., Moqtaderi, H., Hamidi, S. M., Golbabaei, F., Hasanzadeh, M., & Dehghan, S. F. (2025). Magnetic nanoparticles of Nd₂Fe₁₄B prepared by ethanol-assisted wet ball milling technique. Scientific Reports, 15(1), Article 3257. https://doi.org/10.1038/s41598-025-87301-3

Omelyanchik, A., Lamura, G., Peddis, D., & Canepa, F. (2020). Optimization of a Nd-Fe-B permanent magnet configuration for in-vivo drug delivery experiments. Journal of Magnetism and Magnetic Materials, 522, Article 167491. https://doi.org/10.1016/j.jmmm.2020.167491

Ouyang, Y., Qiu, R., Xiao, Y., Shi, Z., Hu, S., Zhang, Y., Chen, M., & Wang, P. (2019). Magnetic fluid based on mussel inspired chemistry as corrosion-resistant coating of Nd-Fe-B magnetic material. Chemical Engineering Journal, 368, 331-339. https://doi.org/10.1016/j.cej.2019.02.126

Périgo, E. A., Silva, S. C., De Sousa, E. M. B., Freitas, A. A., Cohen, R., Nagamine, L. C. C. M., Takiishi, H., & Landgraf, F. J. G. (2012). Properties of nanoparticles prepared from Nd-Fe-B-based compound for magnetic hyperthermia application. Nanotechnology, 23(17), Article 175704. https://doi.org/10.1088/0957-4484/23/17/175704

Pich, A., Bhattacharya, S., Ghosh, A., & Adler, H. (2005). Composite magnetic particles: 2. Encapsulation of iron oxide by surfactant-free emulsion polymerization. Polymer, 46(13), 4596-4603. https://doi.org/10.1016/j.polymer.2005.01.017

Popa, O., Dorolti, E., Borodi, G., Marcu, G., Coldea, M., & Turcu, R. (2013). The influence of milling and annealing on the structural and magnetic behavior of Nd₂Fe₁₄B/α-Fe magnetic nanocomposite. Journal of Alloys and Compounds, 574, 496-501.

Rahimi, H., Ghasemi, A., Mozaffarinia, R., & Tavoosi, M. (2017). Magnetic properties and magnetization reversal mechanism of Nd-Fe-B nanoparticles synthesized by a sol-gel method. Journal of Magnetism and Magnetic Materials, 444, 111-118. https://doi.org/10.1016/j.jmmm.2017.08.011

Saritas, E. U., Goodwill, P. W., Croft, L. R., Konkle, J. J., Lu, K., Zheng, B., & Conolly, S. M. (2012). Magnetic particle imaging (MPI) for NMR and MRI researchers. Journal of Magnetic Resonance, 229, 116-126. https://doi.org/10.1016/j.jmr.2012.11.029

Savchenko, A. G., Menushenkov, V. P., Plastinin, A. Y., Zhukov, A. A., & Kuznetsov, P. A. (2018). Phase composition and magnetic properties of Nd₂Fe₁₄B/α-Fe nanocomposites prepared by mechanical alloying. Russian Metallurgy (Metally), 2018(4), 354-358. https://doi.org/10.1134/S0036029518040134

Schultz, L., Wecker, J., & Hellstern, E. (1987). Formation and properties of Nd-Fe-B prepared by mechanical alloying and solid-state reaction. Journal of Applied Physics, 61(8), 3583-3585. https://doi.org/10.1063/1.338708

Sepehri-Amin, H., Ohkubo, T., Gruber, M., Schrefl, T., & Hono, K. (2014). Micromagnetic simulations on the grain size dependence of coercivity in anisotropic Nd-Fe-B sintered magnets. Scripta Materialia, 89, 29-32. https://doi.org/10.1016/j.scriptamat.2014.06.020

Shen, L., Fan, M., Zhao, K., Qiu, M., & Tian, Z. (2018). Preparation and properties of nanocomposite coatings on sintered Nd-Fe-B magnets. Materials Research Express, 5(8), Article 086401. https://doi.org/10.1088/2053-1591/aad121

Suryanarayana, C. (2010). Synthesis of nanocomposites by mechanical alloying. Journal of Alloys and Compounds, 509(Suppl. 1), S229-S234. https://doi.org/10.1016/j.jallcom.2010.09.063

Tung, D. K., Manh, D. H., Phong, P. T., Phong, L. T. H., Dai, N. V., Nam, D. N. H., & Phuc, N. X. (2015). Structural and magnetic properties of mechanically alloyed Fe₅₀Co₅₀ nanoparticles. Journal of Alloys and Compounds, 640, 34-38. https://doi.org/10.1016/j.jallcom.2015.04.022

Wu, K., Yao, Y., & Klik, I. (1997). Electrical and magnetic properties of Nd-Fe-B films. Applied Surface Science, 113-114, 174-177. https://doi.org/10.1016/s0169-4332(96)00843-4

Yang, C., Ren, B., Wang, D., & Tang, Q. (2019). Synthesis of Nano-Fe@Nd-Fe-B/AC magnetic catalytic particle electrodes and application in the degradation of 2,4,6-trichlorophenol by electro-assisted peroxydisulfate process. Environmental Technology, 41(19), 2464-2477. https://doi.org/10.1080/09593330.2019.1567826

Yang, H., Duan, L., Zhang, P., Xu, G., Cui, J., Lv, J., Sun, W., Li, B., Wang, D., & Wu, Y. (2022). Corrosion resistance of functionalized carbon nanotubes enhanced epoxy coatings on sintered Nd-Fe-B magnets. Journal of Coatings Technology and Research, 19(5), 1317-1329. https://doi.org/10.1007/s11998-022-00641-x

Zhang, J., Wu, W., Meng, F., Ding, H., & Dong, J. (2018). Sol-gel-based chemical synthesis of Nd-Fe-B hard magnetic nanoparticles. Modern Physics Letters B, 32(34n36), Article 1840070. https://doi.org/10.1142/s0217984918400705

Zhou, X., Tian, Y., Yu, H., Zhang, H., Zhong, X., & Liu, Z. (2019). Synthesis of hard magnetic Nd-Fe-B composite particles by recycling the waste using microwave assisted auto-combustion and reduction method. Waste Management, 87, 645-651. https://doi.org/10.1016/j.wasman.2019.02.050

Downloads

Published

2026-06-26

How to Cite

Bellek, M., Kavak, S., & Ağaoğulları, D. (2026). Mechanically Alloyed Nd-Fe-B Nanoparticles with Graphitic Carbon Shell: Synthesis, Characterization and Magnetic Properties. Journal of Defence and Security Industries: Strategy and Technology, 1(2), 177–200. https://doi.org/10.65834/jdsi.12.46