Comparative Effects of Cold Plasma and Thermal Annealing on the Structural and Morphological Properties of Nickel and Iron Oxide Coatings
Abstract
This study comprehensively investigates and compares the effects of Cold Atmospheric Plasma (CAP) treatment as a potential alternative to thermal annealing on the structural and morphological properties of two distinct thin films: nickel (Ni) and iron oxide (FeₓOᵧ), both electrochemically deposited on ITO substrates. Characterization via X-ray diffraction (XRD) and atomic force microscopy (AFM) revealed that the material's nature dictates its response to post-processing. For nickel, short-duration CAP exposure (2.5-5 min) optimally enhanced crystallinity and surface smoothness by reducing grain size and roughness, while longer exposures led to oxidation and increased roughness. Conversely, for iron oxide, even brief CAP treatment initiated a transformation from a monocrystalline to a polycrystalline structure, forming a mixture of phases (Fe₃O₄, γ-Fe₂O₃). The smoothest iron oxide surface was achieved after 5-10 minutes of CAP, with excessive exposure (15 min) causing surface damage. Thermal annealing proved superior for nickel at 200 oC, yielding the smallest grains and smoothest surface. However, it was inadequate for optimal iron oxide crystallization. This work establishes CAP as a rapid, energy-efficient alternative to annealing, with its optimal parameters being highly material-specific, crucial for tailoring functional coatings in catalysis and sensing.
Downloads
References
M. Gavahian, and P.J. Cullen, "Cold Plasma as an Emerging Technique for Mycotoxin-Free Food: Efficacy," Mechanisms, and Trends. Food Reviews International, 36, 193–214 (2019). https://doi.org/10.1080/87559129.2019.1630638
N. Yasoob, K. Khaleel, and H. Murbat, "Study of the Effect of Cold Plasma on the Reproductive Endocrinology of Male Rats," Plant archives, 20, 526–531 (2020).
G.A. ul J. A. ul Sattar, A.N. Yasoob, "Synthesis and Characterization of Silicon Nanoparticles by Argon Plasma Jet Technique and Its Antibacterial S. Aureus Activity," BioNanoScience, 15, 202 (2025). https://doi.org/10.1007/s12668-025-01806-9
Y. Shi, Q. Shu, P.K. Liaw, et al., "Effect of annealing on mechanical and thermoelectric properties of a Al2CoCrFeNi high-entropy alloy," Materials & design, 213, 110313–110313 (2022). https://doi.org/10.1016/j.matdes.2021.110313
A.B. El-Bediwi, E. Kashita, and S.M.M. Salman, "Influence of Annealing on Creep Indentation, Surface Properties and Electrochemical Corrosion Behavior of Ni-Cr Based Dental Alloy," International Journal of Applied Sciences and Biotechnology 5, 366–374 (2017). https://doi.org/10.3126/ijasbt.v5i3.18295
M. Pita, and L. Lebea, "Effect of Annealing on the Microstructure, Hardness, Electrical Conductivity, and Corrosion of Copper Material before Accumulative Roll Bonding Processes," Journal of Engineering, 2022, 1–8 (2022). https://doi.org/10.1155/2022/6963417
J. Butt, H. Afsharnia, A.Alam, and V. Mohaghegh, "Effect of Different Annealing Methods on ULTEM 9085 Parts Manufactured by Material Extrusion," Journal of Manufacturing and Materials Processing, 8, 258–258 (2024). https://doi.org/10.3390/jmmp8060258
G.M. Alonzo-Medina, A. González-González, J.L. Sacedón, and A.I. Oliva, "Understanding the thermal annealing process on metallic thin films," IOP Conference Series: Materials Science and Engineering, 45, 012013 (2013). https://doi.org/10.1088/1757-899x/45/1/012013
R. Wang, Z. Xia, X. Kong, et al., "Etching and annealing treatment to improve the plasma-deposited SiOx film adhesion force," Surface and Coatings Technology, 427, 127840 (2021). https://doi.org/10.1016/j.surfcoat.2021.127840
N. Shota, T. Tsutsumi, I. Sakata, and M. Hori, "Plasma processing and annealing for defect management at SiO2/Si interface," Journal of Vacuum Science & Technology B Nanotechnology and Microelectronics Materials Processing Measurement and Phenomena, 41, (2023). https://doi.org/10.1116/6.0002822
W. Kaczorowski, W. Szymanski, D. Batory, and P. Niedzielski, "Effect of plasma treatment on the surface properties of polydimethylsiloxane," Journal of Applied Polymer Science, 132, (2014). https://doi.org/10.1002/app.41635
O.V. Byrka, S.S. Herashchenko, V.A. Makhlai, et al., "Modification and Alloying Effects In Eurofer Steel Under Powerful Pulsed Plasma Impacts," Problems of Atomic Science and Technology, 191–194 (2021). https://doi.org/10.46813/2021-134-191
Y. Xu, Y. Zhang, T. He, et al., "The Effects of Thermal and Atmospheric Pressure Radio Frequency Plasma Annealing in the Crystallization of TiO2 Thin Films," Coatings, 9, 357–357 (2019). https://doi.org/10.3390/coatings9060357
O. Kylián, "Atmospheric Pressure Plasma Treatment of Materials," in: Meeting abstracts/Meeting abstracts (Electrochemical Society CD-ROM) MA2022-02, (2022), pp.886–886. https://doi.org/10.1149/ma2022-0219886mtgabs
N.A. Yasoob, "Verification and Demonstration of the Ability of Plasma Generated from Dielectric Barrier Discharge to Oxidize," Baghdad Science Journal, 22, 1295-1303 (2024). https://doi.org/10.21123/bsj.2024.11217
R. Pernica, M. Klíma, P. Londák, and P. Fiala, "Modification of Insulating Properties of Surfaces of Dielectric High-Voltage Devices Using Plasma," Applied Sciences, 14, 4399 (2024). https://doi.org/10.3390/app14114399
T. Vopát, Š. Podhorský, M. Kuruc, et al.," Advanced approach of forming cutting edge radii on cemented carbide cutting tools using plasma discharges in electrolyte," Journal of Manufacturing Processes, 120, 778–794 (2024). https://doi.org/10.1016/j.jmapro.2024.04.028
D. Ries, E. Robert, S. Dozias, et al., "Characterisation of plasma sources for biomedical applications," International Plasma Chemistry Society, 5–8 (2011).
S.K. Sharma, and A. Sharma, "Sterilization of Microorganisms Contaminated Surfaces and its Treatment with Dielectric Barrier Discharge Plasma," Transactions of the Indian National Academy of Engineering, 5, 1 (2020). https://doi.org/10.1007/s41403-020-00124-8
X. Sun, B. Zang, and B. Sun, "Surface Modification of Polyethylene in Dielectric Barrier Discharge (DBD) Plasma under Atmospheric-Pressure," IJEIR, 5, 164–167 (2016).
O. Polonskyi, T. Hartig, J.R. Uzarski, and M.J. Gordon, "Precise localization of DBD plasma streamers using topographically patterned insulators for maskless structural and chemical modification of surfaces," Applied Physics Letters, 119, 211601 (2021). https://doi.org/10.1063/5.0071460
W. Zhang, X. Xu, F. Wei, et al., "Influence of Dielectric Barrier Discharge Treatment on Surface Structure of Polyoxymethylene Fiber and Interfacial Interaction with Cement," Materials, 11, 1873 (2018). https://doi.org/10.3390/ma11101873
C. Sawangrat, P. Thipchai, K. Kaewapai, et al., "Surface Modification and Mechanical Properties Improvement of Bamboo Fibers Using Dielectric Barrier Discharge Plasma Treatment," Polymers, 15, 1711 (2023). https://doi.org/10.3390/polym15071711
R.W. Cairns, and E. Ott, "X-Ray Studies of the System Nickel—Oxygen—Water. I. Nickelous Oxide and Hydroxide," Journal of the American Chemical Society, 55, 527–533 (1933). https://doi.org/10.1021/ja01329a013
A. Jumaa, W. Aziz, and M. Abid, "Effect of molar concentration of iron(III) chloride on activity of prepared iron oxide nano-particles for degradation methylene blue," in: 2nd International Conference For Engineering Sciences And Information Technology (Esit 2022), (ESIT2022 Conference Proceedings, (2024).
S.H. Choi, J. Kim, and Y.S. Yoon, "Effect of plasma immersion on crystallinity of V2O5 film grown by dc reactive sputtering at room temperature," Thin Solid Films, 493, 1–5 (2005). https://doi.org/10.1016/j.tsf.2004.07.057
M. Jenko, M. Godec, A. Kocijan, et al., "A new route to biocompatible Nitinol based on a rapid treatment with H2/O2 gaseous plasma," Applied Surface Science, 473, 976–984 (2018). https://doi.org/10.1016/j.apsusc.2018.12.140
F. Hajakbari, S. Rashvand, and A. Hojabri, "Effect of plasma oxidation parameters on physical properties of nanocrystalline nickel oxide thin films grown by two-step method: DC sputtering and plasma oxidation," Journal of theoretical and applied physics, 13, 365–373 (2019). https://doi.org/10.1007/s40094-019-00350-8
N. Ahmed, W. Luo, R. Zhao, et al., "Role of Plasma in Catalyst Preparation and Modification for Oxygen Evolution Reaction," Precision Chemistry, 3, (2024). https://doi.org/10.1021/prechem.4c00075
P. Chytrosz-Wrobel, M. Golda-Cepa, E. Stodolak-Zych, et al., "Effect of oxygen plasma-treatment on surface functional groups, wettability, and nanotopography features of medically relevant polymers with various crystallinities," Applied surface science advances, 18, 100497–100497 (2023). https://doi.org/10.1016/j.apsadv.2023.100497
H. Abdel-Khalek, M.I. El-Samahi, and A.M. El-Mahalawy, "Plasma impact on structural, morphological and optical properties of copper acetylacetonate thin films," Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, 199, 356–366 (2018). https://doi.org/10.1016/j.saa.2018.04.001
L. Vivet, R. Benoit, M.F. Falzon, et al., "XPS, ToF SIMS and wettability analyses on Ni surfaces after Ar-H2 RF plasma treatment: An efficient and optimized plasma treatment approach," Surface & Coatings Technology, 398, 126094–126094 (2020). https://doi.org/10.1016/j.surfcoat.2020.126094
M. Quaas, O. Ivanova, C.A. Helm, and H. Wulff, "Influence of reactive plasmas on thin nickel films," Oldenbourg Wissenschaftsverlag eBooks, 27, 295–302 (2008). https://doi.org/10.1524/9783486992564-036
K.N. Pandiyaraj, M. Karuppusamy, P. Jayamurugan, et al., "Iron oxide nanoparticles (IONPs) synthesized via a novel non-thermal atmospheric pressure plasma-assisted electrolysis: Physicochemical characterization and cytocompatibility evaluation," Advanced Powder Technology, 35, 104441 (2024). https://doi.org/10.1016/j.apt.2024.104441
M. Serhan, D. Jackemeyer, M. Long, et al., "Total Iron Measurement in Human Serum With a Novel Smartphone-Based Assay," IEEE Journal of Translational Engineering in Health and Medicine, 8, 1–9 (2020). https://doi.org/10.1109/jtehm.2020.3005308
V. Stranak, Z. Hubicka, M. Cada, et al., "Influence of reactive oxygen species during deposition of iron oxide films by high power impulse magnetron sputtering," Journal of physics D, Applied physics, 51, 095205–095205 (2018). https://doi.org/10.1088/1361-6463/aaa9e6
W.J. Aziz, Aya Jumaa, and M.A. Abid, "Effect of variation biomass on the properties of iron oxide NPs for hydrolysis of methylene blue dye," Journal of Physics Conference Series, 2322, 012086–012086 (2022). https://doi.org/10.1088/1742-6596/2322/1/012086
M. Chabane, C. Melkaoui, N. Ferrah, et al., "Synthesis and Evaluation of Polyacrylamide Based Filter Pellets Incorporating GAC, Iron Oxide, Zinc Oxide, and Kaolin for Chromium and Nickel Water Remediation," Revue des composites et des matériaux avancés, 34, 221–232 (2024). https://doi.org/10.18280/rcma.340212
Copyright (c) 2026 Aya Jumaa, Duha K. Harfesh, A.N. Yasoob, Hamid H. Murbat
This work is licensed under a Creative Commons Attribution 4.0 International License.
Authors who publish with this journal agree to the following terms:
- Authors retain copyright and grant the journal right of first publication with the work simultaneously licensed under a Creative Commons Attribution License that allows others to share the work with an acknowledgment of the work's authorship and initial publication in this journal.
- Authors are able to enter into separate, additional contractual arrangements for the non-exclusive distribution of the journal's published version of the work (e.g., post it to an institutional repository or publish it in a book), with an acknowledgment of its initial publication in this journal.
- Authors are permitted and encouraged to post their work online (e.g., in institutional repositories or on their website) prior to and during the submission process, as it can lead to productive exchanges, as well as earlier and greater citation of published work (See The Effect of Open Access).
