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Degradation mechanisms of perovskite solar cells under vacuum and one atmosphere of nitrogen

Nature Energy volume 6, pages 977–986 (2021)Cite this article

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An Author Correction to this article was published on 30 March 2022

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Abstract

Extensive studies have focused on improving the operational stability of perovskite solar cells, but few have surveyed the fundamental degradation mechanisms. One aspect overlooked in earlier works is the effect of the atmosphere on device performance during operation. Here we investigate the degradation mechanisms of perovskite solar cells operated under vacuum and under a nitrogen atmosphere using synchrotron radiation-based operando grazing-incidence X-ray scattering methods. Unlike the observations described in previous reports, we find that light-induced phase segregation, lattice shrinkage and morphology deformation occur under vacuum. Under nitrogen, only lattice shrinkage appears during the operation of solar cells, resulting in better device stability. The different behaviour under nitrogen is attributed to a larger energy barrier for lattice distortion and phase segregation. Finally, we find that the migration of excessive PbI2 to the interface between the perovskite and the hole transport layer degrades the performance of devices under vacuum or under nitrogen.

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Fig. 1: Structure and performance of the devices analysed.
Fig. 2: Structure evolution of MAFA PSCs operating in different atmospheres.
Fig. 3: Morphology evolution of MAFA PSCs operating in different atmospheres.
Fig. 4: The thermodynamic driving force of lattice shrinkage and phase segregation.
Fig. 5: Degradation mechanisms of MAFA PSCs under the ISOS-L-1I protocol in different atmospheres.

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Data availability

All data generated or analysed during this study are included in the published article and its supplementary information and source data files. The data can also be found at the following public repository: https://doi.org/10.14459/2021mp1620140.

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Acknowledgements

Financial support from Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) via Germany´s Excellence Strategy – EXC 2089/1 – 390776260 (e-conversion) and via International Research Training Group 2022 Alberta/Technical University of Munich International Graduate School for Environmentally Responsible Functional Materials (ATUMS), as well as from TUM.solar in the context of the Bavarian Collaborative Research Project Solar Technologies Go Hybrid (SolTech) is acknowledged. L.D. thanks the Cambridge Trust and R.G., W.C., L.D., N.L., T.X. and S. Liang acknowledge financial support from the Chinese Scholarship Council (CSC). S.P. acknowledges support from the TUM International Graduate School of Science and Engineering (IGSSE) via the GreenTech Initiative Interface Science for Photovoltaics (ISPV) of the EuroTech Universities, the excellence cluster Nanosystems Initiative Munich (NIM) and the Centre for NanoScience (CeNS). K.J. and S.D.S. acknowledge the Royal Society (UF150033) for funding. We acknowledge the Engineering and Physical Sciences Research Council (EPSRC) for funding (EP/R023980/1). This work was supported by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (HYPERION, grant agreement number 756962).

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Author notes

  1. These authors contributed equally: Renjun Guo, Dan Han, Wei Chen.

Authors and Affiliations

  1. Lehrstuhl für Funktionelle Materialien, Physik-Department, Technische Universität München, Garching, Germany

    Renjun Guo, Wei Chen, Lennart K. Reb, Manuel A. Scheel, Shambhavi Pratap, Nian Li, Shanshan Yin, Tianxiao Xiao, Suzhe Liang, Anna Lena Oechsle, Christian L. Weindl & Peter Müller-Buschbaum

  2. Department Chemie, Ludwig-Maximilians-Universität München, Munich, Germany

    Dan Han & Hubert Ebert

  3. Department of Electrical and Electronic Engineering, Southern University of Science and Technology, Shenzhen, China

    Wei Chen & Kai Wang

  4. Cavendish Laboratory, University of Cambridge, Cambridge, UK

    Linjie Dai, Kangyu Ji, Neil C. Greenham, Samuel D. Stranks & Richard H. Friend

  5. Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, China

    Qiu Xiong & Peng Gao

  6. Department of Chemistry, Nankai University, Tianjin, China

    Saisai Li & Mingjian Yuan

  7. Deutsches Elektronen-Synchrotron (DESY), Hamburg, Germany

    Matthias Schwartzkopf & Stephan V. Roth

  8. Chemical Engineering and Biotechnology, University of Cambridge, Cambridge, UK

    Samuel D. Stranks

  9. Department of Fiber and Polymer Technology, KTH Royal Institute of Technology, Stockholm, Sweden

    Stephan V. Roth

  10. Heinz Maier-Leibnitz-Zentrum, Technische Universität München, Garching, Germany

    Peter Müller-Buschbaum

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  1. Renjun Guo
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Contributions

R.G. provided conceptualization, methodology, formal analysis, investigation, resources, data curation, writing (original draft), project administration and visualization. D.H. and H.E. performed investigation and formal analysis for density function calculation and writing (original draft). W.C. provided resource and investigation for beamtime and supervision. L.D. performed investigation and formal analysis for transient absorption spectra and writing (original draft). K.W. carried out validation and provided resources for the project. K.J. and S.D.S. provided resources and investigation for transient absorption spectra. Q.X. and P.G. contributed resources and investigations for X-ray photoelectron spectroscopy. S. Li and M.Y. provided resources and investigation for Brunauer–Emmett–Teller measurements. L.K.R. contributed software and resources. M.A.S., S.P., S.Y., N.L., T.X. and A.L.O. provided resources and investigation for the beamtime. S. Liang and C.L.W. provided visualizations. N.C.G. and R.F. carried out investigation and formal analysis for transient absorption spectra. M.S. and S.V.R. provided resources, investigation, methodology and curation for the beamtime. P.M.-B. provided conceptualization, funding acquisition, project administration and validation. All authors contributed to writing, review and editing.

Corresponding author

Correspondence to Peter Müller-Buschbaum.

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Competing interests

S.D.S. is a co-founder of Swift Solar. All other authors declare no competing interests.

Additional information

Peer review information Nature Energy thanks Antonino La Magna, Michael McGehee and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Notes 1–7, Figs. 1–14 and Tables 1–13.

Reporting Summary

Supplementary Data 1

Raw data for GIXS evolution.

Supplementary Data 2

Crystallographic data for perovskite.

Source data

Source Data Fig. 1

Numerical source data.

Source Data Fig. 2

Numerical source data.

Source Data Fig. 3

Numerical source data.

Source Data Fig. 4

Numerical source data.

Source Data Fig. 5

Numerical source data.

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Guo, R., Han, D., Chen, W. et al. Degradation mechanisms of perovskite solar cells under vacuum and one atmosphere of nitrogen. Nat Energy 6, 977–986 (2021). https://doi.org/10.1038/s41560-021-00912-8

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