Abstract
The long-term stability of perovskite solar cells remains a challenge. Both the perovskite layer and the device architecture need to endure long-term operation. Here we first use a self-constructed high-throughput screening platform to find perovskite compositions stable under heat and light. Then, we use the most stable perovskite composition to investigate the stability of contact layers in solar cells. We report on the thermal degradation mechanism of transition metal oxide contact (for example, Ta-WOx/NiOx) and propose a bilayer structure consisting of acid-doped polymer stacked on dopant-free polymer as an alternative. The dopant-free polymer provides an acid barrier between the perovskite and the acid-doped polymer. The bilayer structure exhibits stable ohmic contact at elevated temperatures and buffers iodine vapours. The unencapsulated device based on the bilayer contact (with a MgF2 capping layer) retains 99% of its peak efficiency after 1,450 h of continuous operation at 65 °C in a N2 atmosphere under metal-halide lamps. The device also shows negligible hysteresis during the entire ageing period.
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Data availability
All data generated or analysed during this study are included in the article and its Supplementary Information. Supplementary Datasets are provided with this paper.
Code availability
The VBA/MATLAB codes used to analyse the high-throughput data are available as a Supplementary Code file.
References
Bai, S. et al. Planar perovskite solar cells with long-term stability using ionic liquid additives. Nature 571, 245–250 (2019).
Yoo, J. J. et al. Efficient perovskite solar cells via improved carrier management. Nature 590, 587–593 (2021).
Khenkin, M. V. et al. Consensus statement for stability assessment and reporting for perovskite photovoltaics based on ISOS procedures. Nat. Energy 5, 35–49 (2020).
Liu, Z. et al. A holistic approach to interface stabilization for efficient perovskite solar modules with over 2,000-hour operational stability. Nat. Energy 5, 596–604 (2020).
Xiao, K. et al. All-perovskite tandem solar cells with 24.2% certified efficiency and area over 1 cm2 using surface-anchoring zwitterionic antioxidant. Nat. Energy 5, 870–880 (2020).
Wang, Z. et al. High irradiance performance of metal halide perovskites for concentrator photovoltaics. Nat. Energy 3, 855–861 (2018).
Al-Ashouri, A. et al. Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction. Science 370, 1300–1309 (2020).
Hou, Y. et al. Efficient tandem solar cells with solution-processed perovskite on textured crystalline silicon. Science 367, 1135–1140 (2020).
Yang, S. et al. Stabilizing halide perovskite surfaces for solar cell operation with wide-bandgap lead oxysalts. Science 365, 473–478 (2019).
Shi, L. et al. Gas chromatography–mass spectrometry analyses of encapsulated stable perovskite solar cells. Science 368, eaba2412 (2020).
Saliba, M. Perovskite solar cells must come of age. Science 359, 388–389 (2018).
Jeong, M. et al. Stable perovskite solar cells with efficiency exceeding 24.8% and 0.3-V voltage loss. Science 369, 1615–1620 (2021).
Jung, E. H. et al. Efficient, stable and scalable perovskite solar cells using poly(3-hexylthiophene). Nature 567, 511–515 (2019).
Wang, L. et al. A Eu3+–Eu2+ ion redox shuttle imparts operational durability to Pb–I perovskite solar cells. Science 363, 265–270 (2019).
Saliba, M. et al. Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance. Science 354, 206–209 (2016).
Lin, Y. H. et al. A piperidinium salt stabilizes efficient metal-halide perovskite solar cells. Science 369, 96–102 (2020).
Wang, Y. et al. Stabilizing heterostructures of soft perovskite semiconductors. Science 365, 687–691 (2019).
Ishii, T. & Masuda, A. Annual degradation rates of recent crystalline silicon photovoltaic modules. Prog. Photovolt. 25, 953–967 (2017).
PERC technology. LONGi Solar https://en.longi-solar.com/home/products/technology.html (2021).
Jeon, N. J. et al. Compositional engineering of perovskite materials for high-performance solar cells. Nature 517, 476–480 (2015).
Turren-Cruz, S.-H., Hagfeldt, A. & Saliba, M. Methylammonium-free, high-performance, and stable perovskite solar cells on a planar architecture. Science 362, 449–453 (2018).
Ferdani, D. W. et al. Partial cation substitution reduces iodide ion transport in lead iodide perovskite solar cells. Energy Environ. Sci. 12, 2264–2272 (2019).
Juarez-Perez, E. J., Hawash, Z., Raga, S. R., Ono, L. K. & Qi, Y. Thermal degradation of CH3NH3PbI3 perovskite into NH3 and CH3I gases observed by coupled thermogravimetry–mass spectrometry analysis. Energy Environ. Sci. 9, 3406–3410 (2016).
Yi, C. et al. Entropic stabilization of mixed A-cation ABX3metal halide perovskites for high performance perovskite solar cells. Energy Environ. Sci. 9, 656–662 (2016).
Saliba, M. et al. Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency. Energy Environ. Sci. 9, 1989–1994 (2016).
Sun, S. et al. Accelerated development of perovskite-inspired materials via high-throughput synthesis and machine-learning diagnosis. Joule 3, 1437–1451 (2019).
Zhao, Y. et al. Perovskite seeding growth of formamidinium-lead-iodide-based perovskites for efficient and stable solar cells. Nat. Commun. 9, 1607 (2018).
Abdi-Jalebi, M. et al. Maximizing and stabilizing luminescence from halide perovskites with potassium passivation. Nature 555, 497–501 (2018).
Zhao, Y. et al. Strain-activated light-induced halide segregation in mixed-halide perovskite solids. Nat. Commun. 11, 6328 (2020).
Correa-Baena, J. P. et al. Promises and challenges of perovskite solar cells. Science 358, 739–744 (2017).
Zhao, Y. et al. Quantification of light-enhanced ionic transport in lead iodide perovskite thin films and its solar cell applications. Light Sci. Appl. 6, e16243 (2016).
Wu, S. et al. A chemically inert bismuth interlayer enhances long-term stability of inverted perovskite solar cells. Nat. Commun. 10, 1161 (2019).
Peng, J. et al. Nanoscale localized contacts for high fill factors in polymer-passivated perovskite solar cells. Science 371, 390–395 (2021).
Domanski, K. et al. Not all that glitters is gold: metal-migration-induced degradation in perovskite solar cells. ACS Nano 10, 6306–6314 (2016).
Eames, C. et al. Ionic transport in hybrid lead iodide perovskite solar cells. Nat. Commun. 6, 7497 (2015).
Luo, Y. et al. Direct observation of halide migration and its effect on the photoluminescence of methylammonium lead bromide perovskite single crystals. Adv. Mater. 29, 1703451 (2017).
Yu, Z. et al. Simplified interconnection structure based on C60/SnO2-x for all-perovskite tandem solar cells. Nat. Energy 5, 657–665 (2020).
Shao, Y., Xiao, Z., Bi, C., Yuan, Y. & Huang, J. Origin and elimination of photocurrent hysteresis by fullerene passivation in CH3NH3PbI3 planar heterojunction solar cells. Nat. Commun. 5, 5784 (2014).
Jiang, Q. et al. Enhanced electron extraction using SnO2 for high-efficiency planar-structure HC(NH2)2PbI3-based perovskite solar cells. Nat. Energy 2, 16177 (2016).
Hou, Y. et al. A generic interface to reduce the efficiency-stability-cost gap of perovskite solar cells. Science 358, 1192–1198 (2018).
Massonnet, N., Carella, A., de Geyer, A., Faure-Vincent, J. & Simonato, J. P. Metallic behaviour of acid doped highly conductive polymers. Chem. Sci. 6, 412–417 (2015).
Schloemer, T. H. et al. The molybdenum oxide interface limits the high-temperature operational stability of unencapsulated perovskite solar cells. ACS Energy Lett. 5, 2349–2360 (2020).
Christians, J. A. et al. Tailored interfaces of unencapsulated perovskite solar cells for >1,000 hour operational stability. Nat. Energy 3, 68–74 (2018).
Du, X. et al. Elucidating the full potential of OPV materials utilizing a high-throughput robot-based platform and machine learning. Joule 5, 495–506 (2021).
Langner, S. et al. Beyond ternary OPV: high-throughput experimentation and self-driving laboratories optimize multicomponent systems. Adv. Mater. 32, e1907801 (2020).
Zhao, Y. et al. Discovery of temperature-induced stability reversal in perovskites using high-throughput robotic learning. Nat. Commun. 12, 2191 (2021).
Lee, J.-W. et al. Formamidinium and cesium hybridization for photo- and moisture-stable perovskite solar cell. Adv. Energy Mater. 5, 1501310 (2015).
Hauch, J. A., Brabec, C. J., Fabricius, N. & Bergholz, W. Standardization as an instrument to accelerate the development of stable emerging photovoltaic technologies—the IEC TS 62876‐2‐1:2018—technical specification for the stability testing of photovoltaic devices enabled by nanomaterials. Energy Technol. 8, 2000487 (2020).
Panidi, J. et al. Remarkable enhancement of the hole mobility in several organic small-molecules, polymers, and small-molecule:polymer blend transistors by simple admixing of the Lewis acid p-dopant B(C6F5)3. Adv. Sci. 5, 1700290 (2018).
Wang, Z. et al. Efficient ambient-air-stable solar cells with 2D–3D heterostructured butylammonium-caesium-formamidinium lead halide perovskites. Nat. Energy 2, 17135 (2017).
Meng, L. et al. Tailored phase conversion under conjugated polymer enables thermally stable perovskite solar cells with efficiency exceeding 21. J. Am. Chem. Soc. 140, 17255–17262 (2018).
Ren, M., Wang, J., Xie, X., Zhang, J. & Wang, P. Double-helicene-based hole-transporter for perovskite solar cells with 22% efficiency and operation durability. ACS Energy Lett. 4, 2683–2688 (2019).
Arora, N. et al. Perovskite solar cells with CuSCN hole extraction layers yield stabilized efficiencies greater than 20%. Science 358, 768–711 (2017).
Seo, S., Jeong, S., Bae, C., Park, N. G. & Shin, H. Perovskite solar cells with inorganic electron- and hole-transport layers exhibiting long-term (approximately 500 h) stability at 85 °C under continuous 1 sun illumination in ambient air. Adv. Mater. 30, 1801010 (2018).
Acknowledgements
Y. Zhao acknowledges the Alexander von Humboldt Foundation for supporting his scientific research during the postdoctoral period (grant number 1199604). Y. Zhao thanks Y. Lu for the experimental discussion. C.J.B. gratefully acknowledges the financial support through the ‘Aufbruch Bayern’ initiative of the state of Bavaria (EnCN and ‘Solar Factory of the Future’), the Bavarian Initiative ‘Solar Technologies Go Hybrid’ (SolTech) and the SFB 953 (DFG). We acknowledge the grants ‘ELF-PV—Design and Development of Solution-Processed Functional Materials for the Next Generations of PV Technologies’ (no. 44-6521a/20/4) and ‘Solar Factory of the Future’ (FKZ 20.2-3410.5-4-5) by the Bavarian state government and the financial support from the German Research Foundation with grant DFG INST 90/917-1 FUGG and DFG International Graduate School GRK2495/E. J.L. is grateful for the financial support from the Sino-German (CSC-DAAD) Postdoctoral Scholarship Program; J.Z., C.L. and J.W. acknowledge financial support from the China Scholarship Council (CSC).
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Y. Zhao conceived the idea and designed the experiments. Y. Zhao, J.H. and C.J.B. supervised the project. Y. Zhao and J. Z. performed high-throughput experiments. Y. Zhao wrote the codes for data analysis. Y. Zhao, B.L., Y. Zhong and J.L. fabricated the devices, and T.H. characterized the stability. Y. Zhao and J.E. carried out the SEM analyses. O.K. performed XPS characterizations. Y. Zhao wrote the manuscript, and S.L., C.K., A.O., Z.W., J.W., C.L., C.J., N.L., J.H. and C.J.B. contributed to the editing of this manuscript. All authors contributed to the discussion of the work.
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Zhao, Y., Heumueller, T., Zhang, J. et al. A bilayer conducting polymer structure for planar perovskite solar cells with over 1,400 hours operational stability at elevated temperatures. Nat Energy 7, 144–152 (2022). https://doi.org/10.1038/s41560-021-00953-z
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DOI: https://doi.org/10.1038/s41560-021-00953-z
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