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Halogen Redox Shuttle Explains Voltage-Induced Halide Redistribution in Mixed-Halide Perovskite Devices

Cite this: ACS Energy Lett. 2023, 8, 1, 513–520
Publication Date (Web):December 14, 2022
https://doi.org/10.1021/acsenergylett.2c02385
Copyright © 2022 American Chemical Society

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    Abstract

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    Voltage-induced halide segregation greatly limits the optoelectronic applications of mixed-halide perovskite devices, but a mechanistic explanation behind this phenomenon remains unclear. In this work, we use electron microscopy and elemental mapping to directly measure the halide redistribution in mixed-halide perovskite solar cells with quasi-ion-impermeable contact layers under different bias polarities to find iodide and bromide accumulation at the cathode and anode, respectively. This is consistent with a mechanism based on preferential iodide oxidation at the anode, leading to unbalanced Ii+, IX, and BrX fluxes. Importantly, switching the anode from “inert” Au to “active” Ag prevents segregation because Ag oxidation precludes the oxidation of lattice iodide, which suggests employing redox-active additives as a general strategy to suppress halide segregation. Overall, these results show that halide perovskite devices operate as solid-state electrochemical cells when threshold voltages are exceeded, providing fresh insight to understand the impacts of voltage bias on halide perovskite devices.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.2c02385.

    • Experimental details (including materials used in this study, device fabrication methods, and characterizations), long-term voltage biasing tests, EDX spectra, actual voltage drop across the active device and correction methods, and ToF-SIMS measurements (PDF)

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    Cited By

    This article is cited by 7 publications.

    1. Yang Zhou, E Laine Wong, Wojciech Mróz, Giulia Folpini, Samuele Martani, Jesús Jiménez-López, Antonella Treglia, Annamaria Petrozza. Role of Trapped Carriers Dynamics in Operating Lead Halide Wide-Bandgap Perovskite Solar Cells. ACS Energy Letters 2024, 9 (4) , 1666-1673. https://doi.org/10.1021/acsenergylett.4c00488
    2. Yuqin Zou, Johanna Eichhorn, Jiyun Zhang, Fabian A. C. Apfelbeck, Shanshan Yin, Lukas Wolz, Chun-Chao Chen, Ian D. Sharp, Peter Müller-Buschbaum. Microstrain and Crystal Orientation Variation within Naked Triple-Cation Mixed Halide Perovskites under Heat, UV, and Visible Light Exposure. ACS Energy Letters 2024, 9 (2) , 388-399. https://doi.org/10.1021/acsenergylett.3c02617
    3. Hengshan Wang, Yanfeng Yin, Jiao Xu, Jing Li, Yanan Bao, Meiqi An, Lingzhi Tang, Shengye Jin, Wenming Tian, Yiming Yang. Field-Induced Transport Anisotropy in Single-Crystalline All-Inorganic Lead-Halide Perovskite Nanowires. ACS Nano 2023, 17 (23) , 23671-23678. https://doi.org/10.1021/acsnano.3c06944
    4. Jisu Hong, Zhaojian Xu, Dominique Lungwitz, Jonathan Scott, Holly M. Johnson, Yun-Hi Kim, Antoine Kahn, Barry P. Rand. Mitigating Iodine Diffusion by a MoO3–Organic Composite Hole Transport Layer for Stable Perovskite Solar Cells. ACS Energy Letters 2023, 8 (12) , 4984-4992. https://doi.org/10.1021/acsenergylett.3c01873
    5. Mohd Warish, Gaurav Jamwal, Zara Aftab, Nidhi Bhatt, Asad Niazi. Effect of Trap States, Ion Migration, and Interfaces on Carrier Transport in Single-Crystal, Polycrystalline, and Thick Film Devices of Halide Perovskites CH3NH3PbX3 (X = I, Br, Cl). ACS Applied Electronic Materials 2023, 5 (10) , 5432-5445. https://doi.org/10.1021/acsaelm.3c00513
    6. Xinliang Fu, Mei Wang, Yuanzhi Jiang, Xiangyu Guo, Xin Zhao, Changjiu Sun, Li Zhang, Keyu Wei, Hsien-Yi Hsu, Mingjian Yuan. Mixed-Halide Perovskites with Halogen Bond Induced Interlayer Locking Structure for Stable Pure-Red PeLEDs. Nano Letters 2023, 23 (14) , 6465-6473. https://doi.org/10.1021/acs.nanolett.3c01319
    7. Zhaojian Xu, Daniel D. Astridge, Ross A. Kerner, Xinjue Zhong, Junnan Hu, Jisu Hong, Jesse A. Wisch, Kai Zhu, Joseph J. Berry, Antoine Kahn, Alan Sellinger, Barry P. Rand. Origins of Photoluminescence Instabilities at Halide Perovskite/Organic Hole Transport Layer Interfaces. Journal of the American Chemical Society 2023, 145 (21) , 11846-11858. https://doi.org/10.1021/jacs.3c03539

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