Efficient p-i-n-based FAPbI3 perovskite solar cells for scalable solar modules and triple-junction photovoltaics
Hang Hu a b, David B. Ritzer a b, Sophie X. An b, Yang Li a b, Alexander Diercks b, Roja Singh a b, Seyedamir Orooji a b, Qihao Jin b, Paul Fassl a b, Felix Laufer a b, Thomas Feeney a b, Ting Pan a b, Bahram Abdollahi Nejand a b, Ulrich W. Paetzold a b
a Institute of Microstructure Technology (IMT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany.
b Light Technology Institute (LTI), Karlsruhe Institute of Technology (KIT), Engesserstrasse 13, 76131 Karlsruhe, Germany.
Oral, Hang Hu, presentation 033
Publication date: 6th February 2024

Formamidinium lead iodide (FAPbI3) emerges as one of the most promising materials for perovskite solar cells (PSCs) with high power conversion efficiency (PCE) and good stability. However, (i) the scalability lags behind and only a few reports have been dedicated so far towards the scalable processing of FAPbI3 perovskite solar modules; (ii) FAPbI3 has not been applied in multi-junction solar cells and the performance of perovskite–perovskite–silicon triple-junction solar cells lag considerably behind with only a limited number of reports on prototypes. First, this study reports void-free, α-phase, and high-quality FAPbI3 thin films processed via vacuum-assisted growth (VAG) method in p-i-n-based PSCs. VAG eliminates interfacial voids at the buried interface of hole-transport layer (HTL)/FAPbI3, enabling a high PCE of 22.3% for p-i-n-based PSCs. We demonstrate that the voids result in non-radiative recombination loss (i.e., open-circuit voltage (VOC) loss) and poor charge extraction (i.e., low current density (JSC)). An innovative combination of employing methylammonium chloride (MACl) as an additive and applying a moderate N2-flow during the VAG process facilitates blade coating homogeneous large-area FAPbI3 thin films without interfacial voids. As a result, scalable PSCs (0.105 cm2) and mini-modules (aperture area of 12.25 cm2, geometrical fill factor of 96.3%) with PCEs of 20.0% and 18.3% are achieved, respectively. Second, this study addresses significant challenges in processing triple junctions in which the most critical junction is the middle perovskite sub-cell. We present triple-junction perovskite–perovskite–silicon solar cells achieving an unprecedented PCE of 24.4%. Through the optimization of light management for each perovskite sub-cell (with bandgaps of ~1.84 eV and ~1.52 eV for the top and middle cells, respectively), the current generation is maximized to 11.6 mA cm–2. The key to this achievement is the development of a high-performance middle perovskite sub-cell, utilizing a stable pure-α-phase FAPbI3 perovskite thin film that is free of wrinkles, cracks, and pinholes. This enables a high VOC of 2.84 V in the triple-junction architecture. Notably, non-encapsulated triple-junction devices retain up to 96.6% of their initial efficiency when stored in the dark at 85°C for 1081 hours. These are remarkable advances in upscaling FAPbI3-based PSCs and multi-junction PVs.

Financial support from the Initiating and Networking funding of Helmholtz Association HYIG of U.W.P. (VH-NG-1148), the Helmholtz Energy Materials Foundry (HEMF), and Karlsruhe School of Optics and Photonics (KSOP) is gratefully acknowledged. The authors acknowledge the Helmholtz Association (program-oriented funding IV, Materials and Technologies for the Energy Transition, Topic 1: Photovoltaics and Wind Energy, Code: 38.01.02). B.A.N. acknowledges the financial support from the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie (grant agreement no. 840937). H.H. acknowledges the Chinese Scholarship Council (CSC, no. 201808420221) for funding his doctoral research work.

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