Molecular geometry of bulky diammonium cations controls stability and performance in 2D/3D perovskite solar devices
Gustavo de Miguel a, Susana Ramos Terrón a, Juan Pablo Correa-Baena b, Carlo Perini b
a Departamento de Química Física y Termodinámica Aplicada Instituto Químico para la Energía y el Medioambiente (IQUEMA) Universidad de Córdoba Campus de Rabanales Edificio Marie Curie
b School of Materials Science and Engineering Georgia Institute of Technology Atlanta, GA 30332, USA
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
#2Dpero - 2D perovskites: chemical versatility, photophysics and applications
Barcelona, Spain, 2024 March 4th - 8th
Organizers: Claudio Quarti and Yana Vaynzof
Oral, Gustavo de Miguel, presentation 081
DOI: https://doi.org/10.29363/nanoge.matsus.2024.081
Publication date: 18th December 2023

Perovskite-derived two-dimensional (2D) materials are emerging as an excellent combination to the three-dimensional (3D) metal halide perovskites for enhancing its stability.[1] In this 2D/3D approach, bulky ammonium organic cations are deposited on top of the 3D perovskite active layer forming a very thin coating of a low dimensional 2D perovskite.[2] 2D/3D inverted perovskite solar cells (PSCs) have achieved to retain >95% of their initial value after >1000 hours at damp-heat test conditions (85 ºC and 85% RH), while power conversion efficiencies (PCE) above 25% have been recently reported in 2D/3D PSCs.[3]

In this work, we investigate the deposition of two diammonium spacers with similar chemical composition (4,4′-Dithiodianiline, 2S, and 4,4’-ethylenedianiline, ET) but with a totally different molecular geometry on top of a 3D perovskite with Cs0.09FA0.91PbI3 formula to manipulate the efficiency and stability of the PSCs. Our results demonstrate an improved PCE of 21% when using the 2S spacer in opposition to an inferior PCE of 16% in the cells covered with the ET spacer. The stability tests display no loss in the PCE upon constant illumination at RT at the MPPT when using the 2S spacer vs. a significant drop in the PCE for the cells with the ET spacer. This divergent behavior is ascribed to the formation of a parallel oriented layer of a 2D perovskite with the 2S spacer that facilitates the charge extraction in the PSC in opposition to the isotropically layer of a 1D perovskite detected upon addition the ET spacer.

The authors gratefully acknowledge the financial support from PID2020-119209RB-I00 project funded by MCIN/AEI/10.13039/501100011033 by “ERDF A way of making Europe”. They also acknowledge the received funding from the European Union´s Horizon Europe research and innovation programme under grant agreement No 101084422, SUNREY - Boosting SUstaiNability, Reliability and EfficiencY of perovskite PV through novel materials and process engineering (HE-RIA-2021-CL5-D3-101084422)

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