Advantageous mechanochemical synthesis of copper(I) selenide semiconductor, characterization, and properties

doi:10.1007/s11705-021-2066-6

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (3) : 433-442 https://doi.org/10.1007/s11705-021-2066-6

RESEARCH ARTICLE

Advantageous mechanochemical synthesis of copper(I) selenide semiconductor, characterization, and properties

Katarína Gáborová^1,², Marcela Achimovičová¹(

), Michal Hegedüs³, Vladimír Girman⁴, Mária Kaňuchová⁵, Erika Dutková¹

¹. Institute of Geotechnics, Slovak Academy of Sciences, Košice 04001, Slovakia
². Institute of Metallurgy, Faculty of Materials, Metallurgy and Recycling, Technical University, Košice 04201, Slovakia
³. Synthon, s.r.o., Blansko 67801, Czech Republic
⁴. Faculty of Science, Pavol Jozef Šafárik University, Košice 04154, Slovakia
⁵. Institute of Earth Resources, Faculty of Mining, Ecology, Process Control and Geotechnologies, Technical University, Košice 04200, Slovakia

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Abstract

Copper(I) selenide-nanocrystalline semiconductor was synthesized via one-step mechanochemical synthesis after 5 min milling in a planetary ball mill. The kinetics of synthesis was followed by X-ray powder diffraction analysis and specific surface area measurements of milled 2Cu/Se mixtures. The X-ray diffraction confirmed the orthorhombic crystal structure of Cu₂Se with the crystallite size ~25 nm. The surface chemical structure was studied by X-ray photoelectron spectroscopy, whereby the binding energy of the Cu 2p and Se 3d signals corresponded to Cu⁺ and Se^2– oxidation states. Transmission electron microscopy revealed agglomerated nanocrystals and confirmed their orthorhombic structure, as well. The optical properties were studied utilizing ultraviolet-visible spectroscopy and photoluminescence spectroscopy. The direct bandgap energy 3.7 eV indicated a blue-shift phenomenon due to the quantum size effect. This type of Cu₂Se synthesis can be easily adapted to production dimensions using an industrial vibratory mill. The advantages of mechanochemical synthesis represent the potential for inexpensive, environmentally-friendly, and waste-free manufacturing of Cu₂Se.

Keywords Cu₂Se berzelianite nanocrystalline semiconductor mechanochemical synthesis planetary ball mill

Corresponding Author(s): Marcela Achimovičová

Online First Date: 13 July 2021 Issue Date: 24 February 2022

Cite this article:

Katarína Gáborová,Marcela Achimovičová,Michal Hegedüs, et al. Advantageous mechanochemical synthesis of copper(I) selenide semiconductor, characterization, and properties[J]. Front. Chem. Sci. Eng., 2022, 16(3): 433-442.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-021-2066-6
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I3/433

Fig.1 XRPD patterns of 2Cu/Se mixtures milled for 0.5, 1.5, 3, and 5 min.

Fig.2 The graphical LeBail refinement output of the orthorhombic cell parameters against measured data of 2Cu/Se mixtures milled for 5 min.

Tab.1 Indexing of the orthorhombic unit cell along with the relative intensity of Bragg reflections

Fig.3 In-situ monitoring of Cu₂Se mechanochemical synthesis: (a) gas pressure and temperature changes during milling; (b) XRPD pattern of 2Cu/Se mixture milled for 5 min.

Fig.4 Specific surface area, S_A of milled 2Cu/Se mixtures vs. time of mechanochemical synthesis, t_M.

Fig.5 PSD curves of 2Cu/Se mixtures milled for 5 and 7 min.

Fig.6 XPS spectra of mechanochemically synthesized Cu₂Se: (a) Cu 2p; (b) Se 3d.

Fig.7 SEM micrographs of starting reagents: (a) elemental copper and (b) selenium at the same magnification with milled mixtures for (c) 0.5 min and (d) 5 min.

Fig.8 TEM images of (a) agglomerated crystals of Cu₂Se after 5 min of mechanochemical synthesis; (b) detail of Cu₂Se particle imaged at magnification 300 kx; (c) selected area electron diffraction (SAED) pattern of the same crystals.

Fig.9 UV-Vis optical absorption spectrum of Cu₂Se after 5 min of mechanochemical synthesis (Inset: (αhν)² vs. hν plot and the obtained bandgap energy 3.7 eV).

Fig.10 PL spectrum of Cu₂Se product at an excitation wavelength of 480 nm.

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