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Reaction Mechanism of Photocatalytic Hydrogen Production at Water/Tin Halide Perovskite Interfaces

  • Damiano Ricciarelli
    Damiano Ricciarelli
    Department of Chemistry, Biology and Biotechnology, University of Perugia, Via Elce di Sotto 8, 06123 Perugia, Italy
    Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO), Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, 06123 Perugia, Italy
  • Waldemar Kaiser
    Waldemar Kaiser
    Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO), Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, 06123 Perugia, Italy
  • Edoardo Mosconi
    Edoardo Mosconi
    Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO), Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, 06123 Perugia, Italy
  • Julia Wiktor
    Julia Wiktor
    Department of Physics, Chalmers University of Technology, 412 96 Goteborg, Sweden
    More by Julia Wiktor
  • Muhammad Waqar Ashraf
    Muhammad Waqar Ashraf
    Department of Natural Sciences & Mathematics, College of Sciences & Human Studies, Prince Mohammad Bin Fahd University, Al Khobar 31952, Saudi Arabia
  • Lorenzo Malavasi
    Lorenzo Malavasi
    Department of Chemistry and INSTM, Università degli Studi di Pavia, Via Taramelli 16, Pavia 27100, Italy
  • Francesco Ambrosio*
    Francesco Ambrosio
    Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO), Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, 06123 Perugia, Italy
    Department of Chemistry and Biology “A. Zambelli”, University of Salerno, Via Giovanni Paolo II 132, 84084 Fisciano, Salerno, Italy
    [email protected], Istituto Italiano di Tecnologia, Via Pascoli 70/3, 20133 Milano, Italy
    *(F.A.) Email: [email protected]
  • , and 
  • Filippo De Angelis*
    Filippo De Angelis
    Department of Chemistry, Biology and Biotechnology, University of Perugia, Via Elce di Sotto 8, 06123 Perugia, Italy
    Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO), Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, 06123 Perugia, Italy
    Department of Natural Sciences & Mathematics, College of Sciences & Human Studies, Prince Mohammad Bin Fahd University, Al Khobar 31952, Saudi Arabia
    *(F.D.A.) Email: [email protected]
Cite this: ACS Energy Lett. 2022, 7, 4, 1308–1315
Publication Date (Web):March 9, 2022
https://doi.org/10.1021/acsenergylett.2c00122
Copyright © 2022 American Chemical Society
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Supporting Info (1)»

Abstract

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While instability in aqueous environment has long impeded employment of metal halide perovskites for heterogeneous photocatalysis, recent reports have shown that some particular tin halide perovskites (THPs) can be water-stable and active in photocatalytic hydrogen production. To unravel the mechanistic details underlying the photocatalytic activity of THPs, we compare the reactivity of the water-stable and active DMASnBr3 (DMA = dimethylammonium) perovskite against prototypical MASnI3 and MASnBr3 compounds (MA = methylammonium), employing advanced electronic–structure calculations. We find that the binding energy of electron polarons at the surface of THPs, driven by the conduction band energetics, is cardinal for photocatalytic hydrogen reduction. In this framework, the interplay between the A-site cation and halogen is found to play a key role in defining the photoreactivity of the material by tuning the perovskite electronic energy levels. Our study, by elucidating the key steps of the reaction, may assist in development of more stable and efficient materials for photocatalytic hydrogen reduction.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.2c00122.

  • Computational details; electronic structure of MASnI3 vs DMASnBr3 at HSE06-SOC level of theory; PBE/HSE06-SOC band edges; supercells employed to simulate slabs of models A(A′)/B(B′); structures and charge localization for defective slabs; additional references (PDF)

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