GIWAXS characterization of 2D/3D perovskites films prepared in the presence of organic additives and green solvents

Filippo Tavormina^a, Norberto Masciocchi^a, Eleonora Quadrivi^b, Paolo Biagini^b, Riccardo Po'^b, Antonietta Guagliardi^c

^aDipartimento di Scienza e Alta Tecnologia & To.Sca.Lab., Università dell’Insubria, via Valleggio11, 22100 Como, Italy

^bEni - Renewable Energies and Materials Science Research Center

^cIstituto di Cristallografia and To.Sca.Lab, Consiglio Nazionale delle Ricerche, via Valleggio 11, I-22100 Como, Italy

NIPHO
Proceedings of International Conference on Perovskite Thin Film Photovoltaics and Perovskite Photonics and Optoelectronics (NIPHO23)

Pavia, Italy, 2023 May 15th - 16th

Organizers: Giulia Grancini and Silvia Colella

Oral, Filippo Tavormina, presentation 016
DOI: https://doi.org/10.29363/nanoge.nipho.2023.016
Publication date: 3rd April 2023

Hybrid 3D methylammonium (MA) lead halide perovskites (LHP) MAPbI₃ (MAPI) possess excellent optical and photovoltaic (PV) performances, ^[1] but suffer of limited stability in common environmental and working conditions, being ^[2] prone to decomposition favored by heat and moisture. ^[2,3] Large efforts are nowadays spent in the direction of improving the resistance to degradation ^[4] of MAPI active layers in PV devices. Solar cells applications further require the strict control of electron/hole percolation paths and mobility, which are significantly affected by crystal orientation, grain boundaries and other morphological features. ^[5] Recent advances in the fields have been attained by doping these materials with 2D (pseudo)perovskites and/or purely organic additives. ^[6]

Beyond the intrinsic challenges of new hybrid formulations and their optimization, a compelling further aspect to be considered is the environmental and cost sustainability of these semiconductors that are required to combine good performances, environmental stability and green-chemistry approaches.

With this goal in mind, herein we present the characterization of MAPI-based 2D/3D novel formulations in the presence of organic additives, in the form of films from one-pot deposition from a green solvent (DMSO), as a feasible and safe approach toward efficient and sustainable LHP-based PV devices. The formulations rely on the mixed-cation FA_xMA_(1-x)PbI₃ 3D-perovskite (FA = formamidinium), doped with constant amounts of larger organic mono- and di-cations (BA = benzylammonium; BAMB = 1,4-bis-(ammonium-methyl)-benzene; PENDA = 1,5-n-pentane di-ammonium) and increasing amounts of cornstarch in the pristine solution. Films spin-coated on SiO₂/Si substrates are then treated under different mild annealing conditions. The larger organic cation is engaged in the formation of 2D or lower-dimensional perovskites that are expected to impart higher air-stability and impact crystal orientation, whereas cornstarch is useful to tune the rheological and mechanical properties and film homogeneity, and avoids the anti-solvent step. Differently said, addition of cornstarch could make the solution suitable for printable deposition technologies on extended and flexible substrates. _[6] In-situ and ex-situ GIWAXS experiments, performed at Elettra and at ESRF synchrotrons, shed light on the kinetics of crystallization and allow to investigate other distinct effects of dopants and additives on the films texturing. Results will be discussed and correlated to the measured PCE of the films in solar cells device.

References:

[1] Kim, J. Y.; Lee, J.-W.; Jung, H. S.; Shin, H.; Park, N-G. High-Efficiency Perovskite Solar Cells. Chem. Rev., 2020, 120, 7867-7918.

[2] Brunetti, B.; Cavallo, C.; Ciccioli A.; Gigli G.; Latini A. On the Thermal and Thermodynamic (In)Stability of Methylammonium Lead Halide Perovskites. Sci Rep 6, 31896 (2016)

[3] Ciccioli, A.; Latini A. Thermodynamics and the Intrinsic Stability of Lead Halide Perovskites CH3NH3PbX3. J. Phys. Chem. Lett. 2018, 9, 3756-3765

[4] Wang, Z.; Lin, Q.; Chmiel, F. P.; Sakai, N.; Herz, L. M.; Snaith, H. J. Efficient Ambient-Air-Stable Solar Cells with 2D–3D Heterostructured Butylammonium-Caesium-Formamidinium Lead Halide Perovskites. Nature Energy 2017, 2 (9). ‌

[5] Foley, B. J.; Girard, J.; Sorenson, B. A.; Chen, A. Z.; Niezgoda, J. S.; Alpert, M. R.; Harper, A. F.; Smilgies, Detlef-M.; Clancy, P.; Saidi, W. A.; Choi, J. J. Controlling Nucleation, Growth, and Orientation of Metal Halide Perovskite Thin Films with Rationally Selected Additives. Journal of Materials Chemistry A 2016, 5 (1), 113–123.

[6] Giuri, A.; Masi, S.; Listorti, A.; Gigli, G.; Colella, S.; Esposito Corcione, C.; Rizzo, A. Polymeric Rheology Modifier Allows Single-Step Coating of Perovskite Ink for Highly Efficient and Stable Solar Cells. Nano Energy 2018, 54, 400–408.

Acknowledgements:

This work has been performed under the PhD project co-funded by MUR (FSE REACT-EU) and the PE-NEST (PE0000021) project under the National Recovery and Resilience Plan (NRRP), Mission 4 Component 2 Investment 1.3 funded from the European Union - NextGenerationEU.

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