Study of Electrical and Dielectric Behaviors of Copper-Doped Zinc Oxide Ceramic Prepared by Spark Plasma Sintering for Electronic Device Applications

Majdi Benamara; Kais Iben Nassar; Pedro Rivero-Antúnez; Manel Essid; Silvia Soreto Teixeira; Shanyu Zhao; Albert Serrà; Luis Esquivias

doi:10.3390/nano14050402

Study of Electrical and Dielectric Behaviors of Copper-Doped Zinc Oxide Ceramic Prepared by Spark Plasma Sintering for Electronic Device Applications

Nanomaterials (Basel). 2024 Feb 22;14(5):402. doi: 10.3390/nano14050402.

Authors

Majdi Benamara^{1

2}, Kais Iben Nassar^{2

3}, Pedro Rivero-Antúnez^{4

5}, Manel Essid⁶, Silvia Soreto Teixeira², Shanyu Zhao¹, Albert Serrà⁷, Luis Esquivias⁴

Affiliations

¹ Laboratory for Building Energy Materials and Components, Swiss Federal Laboratories for Materials Science and Technology (Empa), 8600 Dübendorf, Switzerland.
² I3N-Aveiro, Department of Physics, University of Aveiro, 3810-193 Aveiro, Portugal.
³ CICECO-Aveiro Institute of Materials, Department of Chemistry, University of Aveiro, Campus Universitário de Santiago, 3810-193 Aveiro, Portugal.
⁴ Departamento de Física de la Materia Condensada, Universidad de Sevilla, 41012 Sevilla, Spain.
⁵ Simidea R&D, European Business and Innovation Centre of Cartagena, 30353 Cartagena, Spain.
⁶ Department of Chemistry, College of Science, King Khalid University, Abha 61413, Saudi Arabia.
⁷ Thin Films and Nanostructures Electrodeposition Group (GE-CPN), Department of Materials Science and Physical Chemistry, University of Barcelona, 08028 Barcelona, Spain.

Abstract

In this study, Cu-doped ZnO aerogel nanoparticles with a 4% copper concentration (Cu4ZO) were synthesized using a sol-gel method, followed by supercritical drying and heat treatment. The subsequent fabrication of Cu4ZO ceramics through Spark Plasma Sintering (SPS) was characterized by X-ray diffraction (XRD), field-emission gun scanning electron microscopy (FE-SEM) equipped with EDS, and impedance spectroscopy (IS) across a frequency range of 100 Hz to 1 MHz and temperatures from 270 K to 370 K. The SPS-Cu4ZO sample exhibited a hexagonal wurtzite structure with an average crystallite size of approximately 229 ± 10 nm, showcasing a compact structure with discernible pores. The EDS spectrum indicates the presence of the base elements zinc and oxygen with copper like the dopant element. Remarkably, the material displayed distinct electrical properties, featuring high activation energy values of about 0.269 ± 0.021 eV. Complex impedance spectroscopy revealed the impact of temperature on electrical relaxation phenomena, with the Nyquist plot indicating semicircular arc patterns associated with grain boundaries. As temperature increased, a noticeable reduction in the radius of these arcs occurred, coupled with a shift in their center points toward the axis center, suggesting a non-Debye-type relaxation mechanism. Dielectric analyses revealed a temperature-driven evolution of losses, emphasizing the material's conductivity impact. Non-Debye-type behavior, linked to ion diffusion, sheds light on charge storage dynamics. These insights advance potential applications in electronic devices and energy storage.

Keywords: Spark Plasma Sintering; activation energy; copper-doped ZnO; electrical conductivity; electronic device applications; impedance spectroscopy.

Grants and funding

The authors are grateful to i3N (LA/P/0037/2020, UID-B/50025/2020 and UID-P/50025/2020) financed by COMPETE 2020 Program and national funds through the FCT/MEC and FEDER under the PT2020 Partnership Agreement. This work is funded by national funds (OE), through FCT—Fundação para a Ciência e a Tecnologia, I.P., in the scope of the framework contract foreseen in the numbers 4, 5 and 6 of article 23, of the Decree-Law 57/2016, of August 29, changed by Law 57/2017, of July 19. S.R.