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    Spacer Engineering of Diammonium‐Based 2D Perovskites toward Efficient and Stable 2D/3D Heterostructure Perovskite Solar Cells

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    aenm.202102973.pdf
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    Description:
    Final Accepted Manuscript
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    Author
    Niu, Tianqi
    Xie, Yue‐Min
    Xue, Qifan
    Xun, Sangni
    Yao, Qin
    Zhen, Fuchao
    Yan, Wenbo
    Li, Hong
    Brédas, Jean‐Luc
    Yip, Hin‐Lap
    Cao, Yong
    Show allShow less
    Affiliation
    Department of Chemistry and Biochemistry, The University of Arizona
    Issue Date
    2021-10-31
    Keywords
    2D/3D heterostructure
    high-performance
    perovskite solar cells
    spacer engineering
    
    Metadata
    Show full item record
    Publisher
    Wiley
    Citation
    Niu, T., Xie, Y.-M., Xue, Q., Xun, S., Yao, Q., Zhen, F., Yan, W., Li, H., Brédas, J.-L., Yip, H.-L., & Cao, Y. (2021). Spacer Engineering of Diammonium-Based 2D Perovskites toward Efficient and Stable 2D/3D Heterostructure Perovskite Solar Cells. Advanced Energy Materials.
    Journal
    Advanced Energy Materials
    Rights
    Copyright © 2021 Wiley-VCH GmbH
    Collection Information
    This item from the UA Faculty Publications collection is made available by the University of Arizona with support from the University of Arizona Libraries. If you have questions, please contact us at repository@u.library.arizona.edu.
    Abstract
    Perovskite solar cells (PSCs) based on 2D/3D heterostructures show great potential to combine the advantages of the high efficiency of 3D perovskites and the high stability of 2D perovskites. However, an in-depth understanding of the organic-spacer effects on the 2D quantum well (QW) structures and electronic properties at the 2D/3D interfaces is yet to be fully achieved, especially in the case of 2D perovskites based on diammonium spacers/ligands. Here, a series of diammonium spacers is considered for the construct ion 2D/3D perovskite heterostructures. It is found that the chemical structure and concentration of the spacers can dramatically affect the characteristics of the 2D capping layers, including their phase purity and orientation. Density functional theory calculations indicate that the spacer modifications can induce shifts in the energy-level alignments at the 2D/3D interfaces and therefore influence the charge-transfer characteristics. The strong intermolecular interactions between the 2,2-(ethylenedioxy)bis(ethylammonium) (EDBE) cations and inorganic [PbI6]4− slabs facilitate a controlled deposition of a phase-pure QW structure (n = 1) with a horizontal orientation, which leads to better surface passivation and carrier extraction. These benefits endow the EDBE-based 2D/3D devices with a high power conversion efficiency of 22.6% and remarkable environmental stability, highlighting the promise of spacer-chemistry design for high-performance 2D/3D PSCs.
    Note
    12 month embargo; first published: 31 October 2021
    ISSN
    1614-6832
    EISSN
    1614-6840
    DOI
    10.1002/aenm.202102973
    Version
    Final accepted manuscript
    Sponsors
    National Natural Science Foundation of China
    ae974a485f413a2113503eed53cd6c53
    10.1002/aenm.202102973
    Scopus Count
    Collections
    UA Faculty Publications

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