One-Step Blade Coating of Inverted Double-Cation Perovskite Solar Cells from a Green Precursor Solvent

Johannes Küffner^a, Jonas Hanisch^a, Tina Wahl^a, Julia Zillner^a, Erik Ahlswede^a, Michael Powalla^a

^aZentrum für Sonnenenergie‐ und Wasserstoff‐Forschung Baden‐Württemberg (ZSW) Stuttgart, Germany, Meitnerstraße, 1, Stuttgart, Germany

International Conference on Hybrid and Organic Photovoltaics
Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)

Online, Spain, 2021 May 24th - 28th

Organizers: Marina Freitag, Feng Gao and Sam Stranks

Oral, Johannes Küffner, presentation 031
Publication date: 11th May 2021

Lab-scale perovskite solar cells (PSCs) have recently reached power conversion efficiencies (PCEs) of up to 25.5%[1] almost exclusively fabricated from precursor solutions containing harmful and polluting solvents such as dimethylformamide (DMF).

A fully sustainable and green solvent[2] such as pure dimethyl sulfoxide (DMSO) would be more desirable[3], [4] as recently presented by Vidal et al.[5] since DMSO offers the lowest human health and environmental impact compared to all other typical polar aprotic solvents for producing PSCs.[5], [6]

However, utilizing pure DMSO for solution processing via scalable printing techniques implies two main challenges in contrast to DMF or DMF:DMSO mixtures: (i) increased dewetting on the subjacent layer[7], [8] due to the high DMSO surface tension of 42.8 mN m^-1[9] and a high viscosity of 2.0 cP[10] resulting in inhomogeneous perovskite films on large-area;[11] (ii) complex quenching and longer solvent evaporation periods of the wet film before crystallization[12] due to its low vapor pressure and high boiling point of 189 °C.[5]

Here, we report on one-step blade coating methylammonium (MA)-free double-cation perovskite for inverted (p-i-n) PSCs using solely the sustainable precursor solvent DMSO at low processing temperatures. To prevent dewetting of the precursor solution and realize sufficient quenching, we apply a blade coated silicon oxide (SiO₂) nanoparticle (NP) wetting agent at the hole transport layer (HTL)/perovskite interface[13], [14] and gas stream-assisted drying[14], respectively. Trends in perovskite grain size, morphology, crystallinity and elemental composition of samples from both, toxic and green, solvent concepts are compared revealing analogical results. Thus, PSCs with 0.24 cm² active area blade coated from purely DMSO achieve comparable PCE of up to 16.7% versus the ones from a DMF:DMSO mixture (16.9%) and thereby showing that the use of toxic DMF is avoidable. This represents an important step for bringing solution processing of PSCs with environmentally friendly precursor solvents closer to industrial realization and application.

References:

[1] Green, M.; Dunlop, E.; Hohl‐Ebinger, J.; Yoshita, M.; Kopidakis, N.; Hao, X. Solar Cell Efficiency Tables (Version 57). Prog. Photovoltaics Res. Appl. 2021, 29 (1), 3–15.

[2] Capello, C.; Fischer, U.; Hungerbühler, K. What Is a Green Solvent? A Comprehensive Framework for the Environmental Assessment of Solvents. Green Chem. 2007, 9 (9), 927.

[3] Park, N.-G. Green Solvent for Perovskite Solar Cell Production. Nat. Sustain. 2020, 3–4.

[4] Byrne, F. P.; Jin, S.; Paggiola, G.; Petchey, T. H. M.; Clark, J. H.; Farmer, T. J.; Hunt, A. J.; Robert McElroy, C.; Sherwood, J. Tools and Techniques for Solvent Selection: Green Solvent Selection Guides. Sustain. Chem. Process. 2016, 4 (1), 7.

[5] Vidal, R.; Alberola-Borràs, J.-A.; Habisreutinger, S. N.; Gimeno-Molina, J.-L.; Moore, D. T.; Schloemer, T. H.; Mora-Seró, I.; Berry, J. J.; Luther, J. M. Assessing Health and Environmental Impacts of Solvents for Producing Perovskite Solar Cells. Nat. Sustain. 2021, 4 (3), 277–285.

[6] Vidal, R.; Alberola‐Borràs, J.; Sánchez‐Pantoja, N.; Mora‐Seró, I. Comparison of Perovskite Solar Cells with Other Photovoltaics Technologies from the Point of View of Life Cycle Assessment. Adv. Energy Sustain. Res. 2021, 2000088.

[7] Wang, J.; Di Giacomo, F.; Brüls, J.; Gorter, H.; Katsouras, I.; Groen, P.; Janssen, R. A. J.; Andriessen, R.; Galagan, Y. Highly Efficient Perovskite Solar Cells Using Non-Toxic Industry Compatible Solvent System. Sol. RRL 2017, 1 (11), 1700091.

[8] Galagan, Y.; Di Giacomo, F.; Gorter, H.; Kirchner, G.; de Vries, I.; Andriessen, R.; Groen, P. Roll-to-Roll Slot Die Coated Perovskite for Efficient Flexible Solar Cells. Adv. Energy Mater. 2018, 8 (32), 1801935.

[9] Geppert-Rybczyńska, M.; Lehmann, J. K.; Safarov, J.; Heintz, A. Thermodynamic Surface Properties of [BMIm][NTf2] or [EMIm][NTf2] Binary Mixtures with Tetrahydrofuran, Acetonitrile or Dimethylsulfoxide. J. Chem. Thermodyn. 2013, 62, 104–110.

[10] Deng, Y.; Van Brackle, C. H.; Dai, X.; Zhao, J.; Chen, B.; Huang, J. Tailoring Solvent Coordination for High-Speed, Room-Temperature Blading of Perovskite Photovoltaic Films. Sci. Adv. 2019, 5 (12), eaax7537.

[11] Jeong, D.-N.; Lee, D.-K.; Seo, S.; Lim, S. Y.; Zhang, Y.; Shin, H.; Cheong, H.; Park, N.-G. Perovskite Cluster-Containing Solution for Scalable D-Bar Coating toward High-Throughput Perovskite Solar Cells. ACS Energy Lett. 2019, 4 (5), 1189–1195.

[12] Shargaieva, O.; Näsström, H.; Smith, J. A.; Többens, D.; Munir, R.; Unger, E. Hybrid Perovskite Crystallization from Binary Solvent Mixtures: Interplay of Evaporation Rate and Binding Strength of Solvents. Mater. Adv. 2020, 1 (9), 3314–3321.

[13] Schultes, M.; Giesbrecht, N.; Küffner, J.; Ahlswede, E.; Docampo, P.; Bein, T.; Powalla, M. Universal Nanoparticle Wetting Agent for Upscaling Perovskite Solar Cells. ACS Appl. Mater. Interfaces 2019, 11 (13), 12948–12957.

[14] Küffner, J.; Wahl, T.; Schultes, M.; Hanisch, J.; Zillner, J.; Ahlswede, E.; Powalla, M. Nanoparticle Wetting Agent for Gas Stream-Assisted Blade-Coated Inverted Perovskite Solar Cells and Modules. ACS Appl. Mater. Interfaces 2020, 12 (47), 52678–52690.

Acknowledgements:

This work was supported by the Federal Ministry for Economic Affairs and Energy (BMWi) under the contract number 03EE1038A (CAPITANO) and funded under H2020-EU.3.3.2 by the European Commission within the project 850937 (PERCISTAND).

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