Abstract

Organic halide salt passivation is considered to be an essential strategy to reduce defects in state-of-the-art perovskite solar cells (PSCs). This strategy, however, suffers from the inevitable formation of in-plane favored two-dimensional (2D) perovskite layers with impaired charge transport, especially under thermal conditions, impeding photovoltaic performance and device scale-up. To overcome this limitation, we studied the energy barrier of 2D perovskite formation from ortho-, meta- and para-isomers of (phenylene)di(ethylammonium) iodide (PDEAI2) that were designed for tailored defect passivation. Treatment with the most sterically hindered ortho-isomer not only prevents the formation of surficial 2D perovskite film, even at elevated temperatures, but also maximizes the passivation effect on both shallow- and deep-level defects. The ensuing PSCs achieve an efficiency of 23.9% with long-term operational stability (over 1000 h). Importantly, a record efficiency of 21.4% for the perovskite module with an active area of 26 cm2 was achieved.

Highlights

  • Organic halide salt passivation is considered to be an essential strategy to reduce defects in state-of-the-art perovskite solar cells (PSCs)

  • The ortho, meta, and para-isomers of PDEAI2 (Fig. 1a) were prepared and further details are provided in the Supplementary

  • We demonstrate that o-PDEAI2 is an effective passivation agent which affords highly efficient and stable PSCs

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Summary

Introduction

Organic halide salt passivation is considered to be an essential strategy to reduce defects in state-of-the-art perovskite solar cells (PSCs) This strategy, suffers from the inevitable formation of in-plane favored two-dimensional (2D) perovskite layers with impaired charge transport, especially under thermal conditions, impeding photovoltaic performance and device scale-up. The disordered stoichiometric compositions at surfaces, the loss of organic components during thermal annealing, and the heterogeneous polycrystalline nature inevitably generate abundant defects in the solution-processed perovskite films, at surfaces and grain boundaries[5,6,7,8] Such defects incur electronic states in the bandgap of the perovskite and behave as nonradiative recombination centers, which shorten the carrier lifetime and limit the photovoltaic performance[9]. A o-PDEAI2-based perovskite module, with an active area of 26 cm[2], presents a record efficiency of 21.4%

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