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Fundamental Flaw in the Current Construction of the TiO2 Electron Transport Layer of Perovskite Solar Cells and Its Elimination
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    Fundamental Flaw in the Current Construction of the TiO2 Electron Transport Layer of Perovskite Solar Cells and Its Elimination
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    • Yan Yan
      Yan Yan
      Beijing National Laboratory for Molecular Sciences, Key Laboratory of Photochemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, The Chinese Academy of Sciences, Beijing 100190, China
      School of Chemistry and Chemical Engineering, Jiangsu University, No. 301, Xuefu Road, Zhenjiang 212013, China
      The Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, Hamburg 22761, Germany
      More by Yan Yan
    • Cheng Liu
      Cheng Liu
      State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources, North China Electric Power University, Beijing 102206, China
      More by Cheng Liu
    • Yi Yang
      Yi Yang
      State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources, North China Electric Power University, Beijing 102206, China
      More by Yi Yang
    • Guoxiang Hu
      Guoxiang Hu
      Department of Chemistry and Biochemistry, Queens College of the City University of New York, Queens, New York 11367, United States
      More by Guoxiang Hu
    • Vandana Tiwari
      Vandana Tiwari
      The Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, Hamburg 22761, Germany
      Department of Chemistry, University of Hamburg, Martin-Luther-King Platz 6, Hamburg 20146, Germany
    • De-en Jiang
      De-en Jiang
      Department of Chemistry, University of California, Riverside, California 92521, United States
      More by De-en Jiang
    • Wei Peng
      Wei Peng
      Beijing National Laboratory for Molecular Sciences, Key Laboratory of Photochemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, The Chinese Academy of Sciences, Beijing 100190, China
      More by Wei Peng
    • Ajay Jha
      Ajay Jha
      The Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, Hamburg 22761, Germany
      The Rosalind Franklin Institute, Harwell Campus, Didcot, Oxfordshire OX11 0FA, U.K.
      Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot OX11 0QX, U.K.
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    • Hong-Guang Duan
      Hong-Guang Duan
      The Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, Hamburg 22761, Germany
      Institut für Theoretische Physik, Universitat Hamburg, Jungiusstraße 9, Hamburg 20355, Germany
      The Departments of Chemistry and Physics, University of Toronto, 80 Street George Street, Toronto M1C 1A4, Canada
    • Friedjof Tellkamp
      Friedjof Tellkamp
      The Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, Hamburg 22761, Germany
    • Yong Ding
      Yong Ding
      State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources, North China Electric Power University, Beijing 102206, China
      More by Yong Ding
    • Weidong Shi
      Weidong Shi
      School of Chemistry and Chemical Engineering, Jiangsu University, No. 301, Xuefu Road, Zhenjiang 212013, China
      More by Weidong Shi
    • Shouqi Yuan
      Shouqi Yuan
      School of Chemistry and Chemical Engineering, Jiangsu University, No. 301, Xuefu Road, Zhenjiang 212013, China
      More by Shouqi Yuan
    • Dwayne Miller
      Dwayne Miller
      The Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, Hamburg 22761, Germany
      The Departments of Chemistry and Physics, University of Toronto, 80 Street George Street, Toronto M1C 1A4, Canada
    • Wanhong Ma*
      Wanhong Ma
      Beijing National Laboratory for Molecular Sciences, Key Laboratory of Photochemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, The Chinese Academy of Sciences, Beijing 100190, China
      University of Chinese Academy of Sciences, Beijing 100049, China
      *Email: [email protected]
      More by Wanhong Ma
    • Jincai Zhao
      Jincai Zhao
      Beijing National Laboratory for Molecular Sciences, Key Laboratory of Photochemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, The Chinese Academy of Sciences, Beijing 100190, China
      University of Chinese Academy of Sciences, Beijing 100049, China
      More by Jincai Zhao
    Other Access OptionsSupporting Information (1)

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 33, 39371–39378
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    https://doi.org/10.1021/acsami.1c09742
    Published August 15, 2021
    Copyright © 2021 American Chemical Society

    Abstract

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    The top-performing perovskite solar cells (efficiency > 20%) generally rely on the use of a nanocrystal TiO2 electron transport layer (ETL). However, the efficacies and stability of the current stereotypically prepared TiO2 ETLs employing commercially available TiO2 nanocrystal paste are far from their maximum values. As revealed herein, the long-hidden reason for this discrepancy is that acidic protons (∼0.11 wt %) always remain in TiO2 ETLs after high-temperature sintering due to the decomposition of the organic proton solvent (mostly alcohol). These protons readily lead to the formation of Ti–H species upon light irradiation, which act to block the electron transfer at the perovskite/TiO2 interface. Affront this challenge, we introduced a simple deprotonation protocol by adding a small amount of strong proton acceptors (sodium ethoxide or NaOH) into the common TiO2 nanocrystal paste precursor and replicated the high-temperature sintering process, which wiped out nearly all protons in TiO2 ETLs during the sintering process. The use of deprotonated TiO2 ETLs not only promotes the PCE of both MAPbI3-based and FA0.85MA0.15PbI2.55Br0.45-based devices over 20% but also significantly improves the long-term photostability of the target devices upon 1000 h of continuous operation.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.1c09742.

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    This article is cited by 13 publications.

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 33, 39371–39378
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.1c09742
    Published August 15, 2021
    Copyright © 2021 American Chemical Society

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