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2D/3D heterojunction engineering at the buried interface towards high-performance inverted methylammonium-free perovskite solar cells

Nature Energy volume 8, pages 946–955 (2023)Cite this article

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Abstract

The main bottlenecks limiting the photovoltaic performance and stability of inverted perovskite solar cells (PSCs) are trap-assisted non-radiative recombination losses and photochemical degradation at the interface between perovskite and charge-transport layers. We propose a strategy to manipulate the crystallization of methylammonium-free perovskite by incorporating a small amount of 2-aminoindan hydrochloride into the precursor inks. This additive also modulates carrier recombination and extraction dynamics at the buried interface via the formation of a bottom-up two-dimensional/three-dimensional heterojunction. The resultant inverted PSC achieves a power conversion efficiency of 25.12% (certified 24.6%) at laboratory scale (0.09 cm2) and 22.48% at a larger area (1 cm2) with negligible hysteresis. More importantly, the resulting unencapsulated devices show superior operational stability, maintaining >98% of their initial efficiency of >24% after 1,500 hours of continuous maximum power point tracking under simulated AM1.5 illumination. Meanwhile, the encapsulated devices retain >92% of initial performance for 1,200 hours under the damp-heat test (85 °C and 85% relative humidity).

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Fig. 1: Structural characterizations of the bottom-up 2D/3D heterojunction at the buried interface.
Fig. 2: Charge-carrier dynamics.
Fig. 3: Device performance and stability.

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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 that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.

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Acknowledgements

Z.Z. acknowledges funding from the Defense Industrial Technology Development Program (JCKY2017110C0654), Fundamental Research Fund for the Central Universities (2022CDJQY-010) and National Natural Science Foundation of China (grant nos. 11974063 and 61904023). J. Chen acknowledges funding from Support Plan for Overseas Students to Return to China for Entrepreneurship and Innovation (grant no. cx2020003), the Fundamental Research Funds for the Central Universities (grant no. 2020CDJ-LHZZ-074) and Natural Science Foundation of Chongqing (grant no. cstc2020jcyj-msxmX0629). H.Z. acknowledges the funding from Shanghai Pujiang Program (22PJ1401200). M.G. acknowledges funding from the European Union’s Horizon 2020 research and innovation programme GRAPHENE Flagship Core 3 grant agreement no. 881603. X.L. acknowledges the Research Fund of the State Key Laboratory of Solidification Processing (NPU) (grant no. 2021-QZ-02) and the Fundamental Research Funds for the Central Universities (3102019JC005).

Author information

Author notes

  1. These authors contributed equally: Haiyun Li, Cong Zhang, Cheng Gong, Daliang Zhang.

Authors and Affiliations

  1. Key Laboratory of Optoelectronic Technology & Systems (Ministry of Education), Chongqing University, Chongqing, China

    Haiyun Li, Cong Zhang, Cheng Gong, Qixin Zhuang, Ru Li, Jiangzhao Chen & Zhigang Zang

  2. Multi-scale Porous Materials Center, Institute of Advanced Interdisciplinary Studies, Chongqing University, Chongqing, China

    Daliang Zhang, Jingwei Li & Jinfei Zhou

  3. Shanghai Frontiers Science Research Base of Intelligent Optoelectronics and Perception, Institute of Optoelectronics, Department of Materials Science, Fudan University, Shanghai, China

    Hong Zhang & Junhao Chu

  4. SUSTech Energy Institute for Carbon Neutrality, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, China

    Xuemeng Yu, Shaokuan Gong & Xihan Chen

  5. State Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi’an, China

    Jiabao Yang & Xuanhua Li

  6. Institute of High Energy Physics, Chinese Academy of Sciences (CAS), Beijing, China

    Hua Yang

  7. Key Lab of Artificial Micro- and Nano-Structures of Ministry of Education of China, School of Physics and Technology, Wuhan University, Wuhan, China

    Qianqian Lin

  8. Laboratory of Photonics and Interfaces, École Polytechnique Fédérale de Lausanne, Lausanne, Switzerland

    Michael Grätzel

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Contributions

H.L., J. Chen and Z.Z. conceived the project. H.L., C.Z., C.G. and Q.Z. prepared the samples and devices, and performed all other measurement except for TEM, TRS, GIWAXS and time-resolved microwave conductivity measurements. D.Z., J.L. and J.Z. performed TEM measurements. X.Y., S.G. and X.C. conducted TRS measurements. H.Y. carried out GIWAXS measurements. Q.L. performed time-resolved microwave conductivity measurements. H.Z. and J. Chen wrote the first draft of the manuscript. H.L. and R.L. certified the efficiency of the PSCs. J.Y. and X.L. conducted the long-term operational stability measurements. M.G. was involved in the data analysis and wrote the final version of the manuscript. H.Z., X.L., M.G., J. Chen and Z.Z. supervised this project. All authors analysed the data and contributed to the discussions.

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Correspondence to Hong Zhang, Xuanhua Li, Michael Grätzel, Jiangzhao Chen or Zhigang Zang.

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Nature Energy thanks Eline Hutter, Atsushi Wakamiya, Christian Wolff and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Figs. 1–30, Notes 1 and 2 and Tables 1–4.

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Supplementary Data 1

The individual raw data for Supplementary Fig. 19 and Supplementary Table 2.

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The source data for Fig. 3a,f.

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Li, H., Zhang, C., Gong, C. et al. 2D/3D heterojunction engineering at the buried interface towards high-performance inverted methylammonium-free perovskite solar cells. Nat Energy 8, 946–955 (2023). https://doi.org/10.1038/s41560-023-01295-8

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