Abstract
The aim of this research is to elaborate a new lead-free CH3CH2NH3BaCl3 organic–inorganic hybrid perovskite using slow evaporation process at ambient temperature, and to study its structural, microstructural, optical, dielectric, and electrical properties. The X-ray diffraction and Rietveld method analysis exhibit a well crystallized sample in a monoclinic system with the P2/m space group without the presence of a secondary phase. scanning electron microscopy coupled with energy-dispersive X-ray presents a flat surface morphology without impurities or secondary elements, confirming the excellent crystallinity of prepared crystals. Moreover, the Ultraviolet–visible absorption was carried out to identify optical proprieties, that showed a direct bandgap about 4.43 eV. The dielectric measurements present a ferro-paraelectric phase transition with a classic ferroelectric behavior of the material. The electrical properties revealed a non-Debye conduction mechanism, in which the charge carriers require an activation energy around Ea = 0.816 eV.
Graphical abstract
Similar content being viewed by others
Data availability
The authors declare that the data sets generated and/or analyzed during the current study are available from the corresponding author on reasonable request.
References
N.I. Selivanov et al., Hybrid organic-inorganic halide post-perovskite 3-cyanopyridinium lead tribromide for optoelectronic applications. Adv. Funct. Mater. 31(37), 1–8 (2021). https://doi.org/10.1002/adfm.202102338
C. Zhou, H. Lin, S. Lee, M. Chaaban, B. Ma, Organic–inorganic metal halide hybrids beyond perovskites. Mater. Res. Lett. 6(10), 552–569 (2018). https://doi.org/10.1080/21663831.2018.1500951
R. El Mrabet, S. Kassou, O. Tahiri et al., Theoretical and experimental investigations of optical, structural and electronic properties of the lower-dimensional hybrid [NH3-(CH2)10-NH3]ZnCl4. Eur. Phys. J. Plus 131, 369 (2016). https://doi.org/10.1140/epjp/i2016-16369-x
R. El Mrabet, S. Kassou, O. Tahiri, A. Belaaraj, L. El Ammari, M. Saadi, A zero-dimensional hybrid organic-inorganic perovskite ZnCl4 based: synthesis, crystal structure, UV–vis, and electronic properties. J. Cryst. Growth 472, 76–83 (2017). https://doi.org/10.1016/j.jcrysgro.2017.02.026
K. Jemli, H. Diab, F. Lédée, G. Trippé-Allard, D. Garrot, B. Geffroy, J.-S. Lauret, P. Audebert, E. Deleporte, Using low temperature photoluminescence spectroscopy to investigate CH3NH3PbI3 hybrid perovskite degradation. Molecules 21(7), 885 (2016). https://doi.org/10.3390/molecules21070885
A. Varadwaj, P.R. Varadwaj, H.M. Marques, K. Yamashita, The pnictogen bond, together with other non-covalent interactions, in the rational design of one-, two- and three-dimensional organic-inorganic hybrid metal halide perovskite semiconducting materials, and beyond. Int. J. Mol. Sci. 23(15), 8816 (2022). https://doi.org/10.3390/ijms23158816
M. Ettakni et al., Optical and dielectric properties of metal halide perovskites 2D. Bull. Mater. Sci. (2021). https://doi.org/10.1007/s12034-021-02418-1
D. Weber, CH3NH3PbX3, ein Pb(II)-System mit kubischer Perowskitstruktur / CH3NH3PbX3, a Pb(II)-System with Cubic Perovskite Structure. Zeitschrift für Naturforsch. B 33(12), 1443–1445 (1978). https://doi.org/10.1515/znb-1978-1214/html
A. Kojima et al., Organometal halide perovskites as visible-light sensitizers for photovoltaic cells. J. Am. Chem. Soc. 131(17), 6050–6051 (2009). https://doi.org/10.1021/ja809598r
H. Souissi, O. Taktak, M. Khalfa, A. Oueslati, S. Kammoun, Experimental and optical studies of the new organic-inorganic. Opt. Mater. 129, 112513 (2022). https://doi.org/10.1016/j.optmat.2022.112513
M.M. Abdelkader, M. Abdelmohsen, A.I. Aboud, Crystal structure, magnetic susceptibility, dielectric permittivity, and phase transition in a new organic–inorganic hybrid perovskite (n-C8H17NH3)2CoCl4. Chem. Phys. Lett. 770, 138423 (2021). https://doi.org/10.1016/j.cplett.2021.138423
S.H. Kim, A.R. Lim, Structures, phase transitions, thermodynamic properties, and structural dynamics of eco-friendly hybrid perovskite NH3(CH2)3NH3CoCl4 and NH3(CH2)5NH3CoCl4 crystals. Solid State Sci. 131(June), 106927 (2022). https://doi.org/10.1016/j.solidstatesciences.2022.106927
A. Gannouni, H. Louis, T. Roisnel, B.B. Isang, I. Benjamin, R. Kefi, X-ray crystallography, spectral analysis, DFT studies, and molecular docking of (C9H15N3)[CdCl4] hybrid material against methicillin-resistant Staphylococcus aureus (MRSA). Polycycl. Aromat. Compd. (2023). https://doi.org/10.1080/10406638.2023.2169721
S.K. Abdel-aal, A. Ouasri, Crystal structures, hhirshfeld surfaces analysis, infrared and Raman studies of organic-inorganic hybrid perovskite salts NH3(CH2)nNH3MnCl4 (n = 5, 6). J. Solid State Chem. 314(June), 123401 (2022). https://doi.org/10.1016/j.jssc.2022.123401
X.H. Lv, W.Q. Liao, P.F. Li, Z.X. Wang, C.Y. Mao, Y. Zhang, Dielectric and photoluminescence properties of a layered perovskite-type organic-inorganic hybrid phase transition compound: NH3(CH2)5NH3MnCl4. J. Mater. Chem. C 4(9), 1881–1885 (2016). https://doi.org/10.1039/c5tc04114g
N.K. Noel et al., Lead-free organic-inorganic tin halide perovskites for photovoltaic applications. Energy Environ. Sci. 7(9), 3061–3068 (2014). https://doi.org/10.1039/c4ee01076k
R. Kalthoum, M. Ben Bechir, A. Ben Rhaiem, M.H. Dhaou, Optical properties of new organic-inorganic hybrid perovskites (CH3)2NH2CdCl3 and CH3NH3CdCl3 for solar cell applications. Opt. Mater. (2022). https://doi.org/10.1016/j.optmat.2022.112084
S. Soudani, E. Jeanneau, C. Jelsch, F. Lefebvre, C. Ben Nasr, H. Longchambon, Structural, crystal structure, Hirshfeld surface analysis and physicochemical studies of a new chlorocadmate template by 1-(2-hydroxyethyl) piperazine. J. Mol. Struct. 1123, 66–74 (2016). https://doi.org/10.1016/j.molstruc.2016.06.024
K. Azouzi, B. Hamdi, A. Ben Salah, A new organic-inorganic hybrid compound (C7H7N2)2[Cu2Cl6]: synthesis, crystal structure, hirshfeld surface analysis, vibrational and thermal properties. J. Clust. Sci. 28(5), 3021–3034 (2017). https://doi.org/10.1007/s10876-017-1274-1
C. Ayari et al., Synthesis, crystal structure, hirshfeld surface, and physicochemical characterization of new salt Bis (2-ethyl-6-methylanilinium) tetrachloromercurate (II)[C9H14N]2HgCl4. J. Chem. (2021). https://doi.org/10.1155/2021/2857369
C. Ayari et al., A new Zn(II) metal hybrid material of 5-nitrobenzimidazolium organic cation (C7H6N3O2)2[ZnCl4]: elaboration, structure, hirshfeld surface, spectroscopic, molecular docking analysis, electric and dielectric properties. Materials 15(22), 7973 (2022). https://doi.org/10.3390/ma15227973
C. Ben Mohamed, K. Karoui, A. Ben Rhaiem, Optical, structural characterization and dielectric relaxation of [C2H5NH3]2ZnCl4 compound. Phase Trans. 91(11), 1162–1178 (2018). https://doi.org/10.1080/01411594.2018.1521521
L. Zhang, J. Wang, F. Han, S. Mo, F. Long, Y. Gao, Crystal structure and electrical conduction of the new organic-inorganic compound (CH2)2(NH3)2CdI4. J. Mol. Struct. 1156, 450–456 (2018). https://doi.org/10.1016/j.molstruc.2017.11.130
M.S. Lassoued et al., Structural, vibrational and optical properties of a new self assembled organic–inorganic crystal (C4H7N2) [CdCl3(H2O)]. J. Mater. Sci. Mater. Electron. 28(17), 12698–12710 (2017). https://doi.org/10.1007/s10854-017-7095-z
A.R. Lim, S.H. Park, Characterization on lead-free hybrid perovskite [NH3(CH2)5NH3]CuCl4: thermodynamic properties and molecular dynamics. Molecules 27, 4546 (2022). https://doi.org/10.3390/molecules27144546
M. Ben Abdessalem, S. Chkoundali, A. Oueslati, A. Aydi, AC conductivity and phase transition of the BST-BFO ceramic doped with Yb. RSC Adv. 12(42), 27154–27161 (2022). https://doi.org/10.1039/d2ra03371b
R. Kalthoum, M. Ben Bechir, A. Ben Rhaiem, “CH3NH3CdCl3: a promising new lead-free hybrid organic–inorganic perovskite for photovoltaic applications. Phys. E Low-Dimens. Syst. Nanostruct. (2020). https://doi.org/10.1016/j.physe.2020.114235
Z.-L. Xiao, H.-Z. Chen, M.-M. Shi, Wu. Gang, R.-J. Zhou, Z.-S. Yang, M. Wang, B.-Z. Tang, Preparation and characterization of organic–inorganic hybrid perovskite (C4H9NH3)2CuCl4. Mater. Sci. Eng. B 117(3), 313–316 (2005). https://doi.org/10.1016/j.mseb.2004.12.052
M. Khalfa et al., Synthesis, structural and electrical characterization of a new organic inorganic bromide: [(C3H7)4N]2CoBr4. RSC Adv. 12, 2798–2809 (2022). https://doi.org/10.1039/D1RA07965D
B.S. Kusmariya, A. Tiwari, A.P. Mishra, G.A. Naikoo, Theoretical and experimental studies of Cu(II) and Zn(II) coordination compounds with N, O donor bidentate Schiff base ligand containing amino phenol moiety. J. Mol. Struct. 1119, 115–123 (2016). https://doi.org/10.1016/j.molstruc.2016.04.056
A. Kaiba et al., Synthesis, growth, and characterisation of a novel organic–inorganic perovskite-type hybrid system based on glycine. J. Mol. Struct. 1224, 1 (2021). https://doi.org/10.1016/j.molstruc.2020.129008
S. Hermi et al., The coordination behavior of two new complexes, [(C7H10NO2)CdCl3]n (I) and [(C7H9NO2)CuCl2] (II), based on 2,6-dimethanolpyridine; elaboration of the structure and Hirshfeld surface, optical, spectroscopic and thermal analysis. Materials 15(5), 1 (2022). https://doi.org/10.3390/ma15051624
A. Kaiba, F. Al Otaibi, M.H. Geesi, Y. Riadi, T.A. Aljohani, P. Guionneau, A new organic–inorganic hybrid compound (NH3(CH2)C6H4CO2H)[SnCl6]: synthesis, crystal structure, vibrational, optical, magnetic properties and theoretical study. J. Mol. Struct. (2021). https://doi.org/10.1016/j.molstruc.2021.130129
M.H. Mrad, I. Feddaoui, M.S.M. Abdelbaky, S. García-Granda, C. Ben Nasr, Elaboration, crystal structure, characterization and DFT calculation of a new Hg(II) inorganic-organic hybrid salt [C6H16N2O]HgCl4. J. Solid State Chem. (2020). https://doi.org/10.1016/j.jssc.2020.121280
J.A. Alonso, P. Kayser, B.K. Hong, M.C. Álvarez-Galván, F. Fauth, C.A. López, Mechano-chemical synthesis, structural features and optical gap of hybrid CH3NH3CdBr3 perovskite. Materials (2021). https://doi.org/10.3390/ma14206039
A. Filippov, S. Kurakin, O.I. Gnezdilov, O.N. Antzutkin, Effect of magnetic field on diffusion of ethylammonium nitrate—water mixtures confined between polar glass plates. J. Mol. Liq. 274(2020), 45–51 (2019). https://doi.org/10.1016/j.molliq.2018.10.080
I. Dhouib, A. Ouasri, P. Guionneau, S. Pechev, Z. Elaoud, Synthesis, molecular structure, vibrational studies, optical properties and electrical conduction mechanism of the new hybrid compound based on selenate. J. Saudi Chem. Soc. 24(12), 996–1009 (2020). https://doi.org/10.1016/j.jscs.2020.10.007
J. Tauc, Optical properties and electronic structure of amorphous Ge and Si. Mater. Res. Bull. 3(1), 37–46 (1968). https://doi.org/10.1016/0025-5408(68)90023-8
H. Elgahami, J. Lhoste, S. Auduste et al., Organic-inorganic hybrid material [(C2H5)4N]2ZnI4: synthesis, thermal behavior and spectroscopic studies. Res. Sq. (2022). https://doi.org/10.21203/rs.3.rs-1468882/v1
S. Kassou, R. El Mrabet, A. Belaaraj, P. Guionneau, N. Hadi, T. Lamcharfi, Optical and dielectric properties of self-assembled 0D hybrid organic-inorganic insulator. World Acad. Sci. Eng. Technol. Int. J. Math. Comput. Phys. Electr. Comput. Eng. 11(3), 116–120 (2017)
A. Benatia, N. Gouitaa, T. Dine Lamcharfi, F. Abdi, M. Haddad, Effect of calcination temperature and duration on structural and dielectric properties of CaFeO3-δ. Arab. J. Chem. 17(1), 105407 (2024). https://doi.org/10.1016/j.arabjc.2023.105407
M. Daoudy, N. Gouitaa, F.Z. Ahjyaje, T. Dine Lamcharfi, F. Abdi, BZT substitution effect on the characteristics of (1–x) MT – x BZT composite ceramics synthesized by the sol–gel method. Arab. J. Chem. 17(1), 105392 (2024). https://doi.org/10.1016/j.arabjc.2023.105392
M.F. Mostafa, S.S. El-khiyami, S.K. Alal, Structure, thermal, and impedance study of a new organic–inorganic hybrid [(CH2)7(NH3)2]CoCl4. J. Phys. Chem. Solids 118, 6–13 (2018). https://doi.org/10.1016/j.jpcs.2018.02.048
N. Gouitaa, T. Lamcharfi, M.F. Bouayad, F. Abdi, N.S. Echatoui, N. Hadi, Dielectric anomalies of BaTi1-xFexO3 ceramics for x = 0.0 to 0.6 of Fe doping concentration. Asian J. Chem. 29(10), 2143–2148 (2017). https://doi.org/10.14233/ajchem.2017.20653
I. Soudani, K. Ben Brahim, A. Oueslati, H. Slimi, A. Aydi, K. Khirouni, Investigation of structural, morphological, and transport properties of a multifunctional Li-ferrite compound. RSC Adv. 12(29), 18697–18708 (2022). https://doi.org/10.1039/d2ra02757g
M.S. Lassoued, H.H. Osman, M.S.M. Abdelbaky, A. Lassoued, S. Ammar, A.B. Salah, A. Gadri, S. García-Granda, Synthesis, crystal structure, DFT (B3LYP/LanL2DZ) and photoluminescence study of new stanate (IV) based inorganic-organic hybrid. J. Phys. Chem. Solids 121, 177–185 (2018). https://doi.org/10.1016/j.jpcs.2018.05.024
H. Elgahami, W. Trigui, A. Oueslati, F. Hlel, M. Belhouchet, M. Gargouri, Hirshfeld surface, RMN study, optical properties and dielectric behavior of tetrabutylphosphonium tetrachloroantimonate (III) hybrid. J. Iran. Chem. Soc. 18(9), 2473–2482 (2021). https://doi.org/10.1007/s13738-021-02203-1
N. Gouitaa, T. Lamcharfi, M. Bouayad, F. Abdi, N. Hadi, Impedance, modulus and conductivity studies of Fe3+ doped BaTiO3 ceramics prepared by solid state method. J. Mater. Sci. Mater. Electron. 29(8), 6797–6804 (2018). https://doi.org/10.1007/s10854-018-8666-3
I. Gharbi, A. Oueslati, A. Ates, A. Mahmoud, M. Zaghrioui, M. Gargouri, Investigation of structural, morphological, and electrical conductivity study for understanding transport mechanisms of perovskite CH3NH3HgCl3. RSC Adv. 13(15), 10036–10050 (2023). https://doi.org/10.1039/d3ra00671a
N. Gouitaa, F.Z. Ahjyaje, T. Lamcharfi, F. Abdi, M. Haddad, Colossal dielectric constant (CDC) response in 0.5CaTiO3–0.5FeTiO3 composites. J. Mater. Res. 38(9), 2486 (2023). https://doi.org/10.1557/s43578-023-00981-3
N. Gouitaa, F.Z. Ahjyaje, T. Lamcharfi, F. Abdi, M. Haddad, M. Sajieddine, M. Ounacer, Investigation of relaxor and diffuse dielectric phase transitions of Ba1−XBixTi0.8Fe0.2O3 materials. Heliyon (2023). https://doi.org/10.1016/j.heliyon.2023.e16264
K. BenBrahim, M. BenGzaiel, A. Oueslati, M. Gargouri, Electrical conductivity and vibrational studies induced phase transitions in [(C2H5)4N]FeCl4. RSC Adv. 8(71), 40676–40686 (2018). https://doi.org/10.1039/c8ra07671e
A.K. Jonscher, The ‘universal’ dielectric response. Nature 267, 673–679 (1977). https://doi.org/10.1038/267673a0
K. Ben Brahim et al., Organic-inorganic interactions revealed by Raman spectroscopy during reversible phase transitions in semiconducting [(C2H5)4N]FeCl4. RSC Adv. 11(30), 18651–18660 (2021). https://doi.org/10.1039/d1ra02475b
Acknowledgments
This work was been carried out in Signals, Systems and Components Laboratory, at University Sidi Mohamed Ben Abdellah, Fez, Morocco. The authors Acknowledge the Innovation Center of the university for their support and assistance in processing the sample utilized in this study. We sincerely thank the reviewers for their considerate corrections and valuable criticisms during the evaluation of the manuscript.
Funding
There is no funding provided for this work.
Author information
Authors and Affiliations
Contributions
MD: Formal analysis, validation, and writing of the original version. NG: Formal analysis, validation, and writing of the original version. FZA: Formal analysis, validation, and writing of the original version. T-DL: Formal analysis, validation, and writing of the original version. FA: Formal analysis, validation, and writing of the original version.
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Daoudy, M., Gouitaa, N., Ahjyaje, F.Z. et al. Synthesis, structural study, optical, dielectric, and electrical properties of a new lead-free C2H5NH3BaCl3 organic–inorganic hybrid perovskite. Journal of Materials Research (2024). https://doi.org/10.1557/s43578-024-01318-4
Received:
Accepted:
Published:
DOI: https://doi.org/10.1557/s43578-024-01318-4