Herein, we reveal for the first time a comprehensive mechanism of poorly investigated electrochemical decomposition of CH3NH3PbI3 using a set of microscopy techniques (optical, AFM, PL) and ToF-SIMS. We demonstrate that applied electric bias induces the oxidation of I– to I2, which remains trapped in the film in the form of polyiodides, and hence, the process can be conceivably reversed by reduction. On the contrary, reduction of organic methylammonium cation produces volatile products, which leave the film and thus make the degradation irreversible. Our results lead to a paradigm change when considering design principles for improving the stability of complex lead halide materials as those featuring organic cations rather than halide anions as the most electric field-sensitive components. Suppressing the electrochemical degradation of complex lead halides represents a crucial challenge, which should be addressed in order to bring the operational stability of perovskite photovoltaics to commercially interesting benchmarks.

Methylammonium lead triiodide (CH3NH3PbI3/MAPbI3) is the most intensively explored perovskite light-absorbing material for hybrid organic–inorganic perovskite photovoltaics due to its unique optoelectronic properties and advantages. This includes tunable bandgap, a higher absorption coefficient than conventional materials used in photovoltaics, ease of manufacturing due to solution processability, and low fabrication costs. In addition, the MAPbI3 absorber layer provides one of the highest open-circuit voltages (Voc), low Voc loss/deficit, and low exciton binding energy, resulting in better charge transport with decent charge carrier mobilities and long diffusion lengths of charge carriers, making it a suitable candidate for photovoltaic applications. Unfortunately, MAPbI3 suffers from poor photochemical stability, which is the main problem to commercialize MAPbI3-based perovskite solar cells (PSCs). However, researchers frequently adopt additive engineering to overcome the issue of poor stability. Therefore, in this review, we have classified additives as organic and inorganic additives. Organic additives are subclassified based on functional groups associated with N/O/S donor atoms; whereas, inorganic additives are subcategorized as metals and non-metal halide salts. Further, we discussed their role and mechanism in terms of improving the performance and stability of MAPbI3-based PSCs. In addition, we scrutinized the additive influence on the morphology and optoelectronic properties to gain a deeper understanding of the crosslinking mechanism into the MAPbI3 framework. Our review aims to help the research community, by providing a glance of the advancement in additive engineering for the MAPbI3 light-absorbing layer, so that new additives can be designed and experimented with to overcome stability challenges. This, in turn, might pave the way for wide scale commercial use.

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Perovskites have already shown potential as active layers in photovoltaic applications. Furthermore, a low-cost and simple solution processing technology allows perovskites to be used in flexible and printed electronics. Perovskite solar cells (PSC) with a back-contact (BC) structure, in which the electrode system is based on a quasi-interdigitated back-contact (QIBC) design, promise to increase the power conversion efficiency (PCE) of devices beyond those that can be obtained using PSCs with a traditional sandwich structure. While the spin-coating technique is used to deposit the perovskite layer of lab-scale BC PSCs, the application of large-area printing techniques to deposit the perovskite layer of such devices is yet to be explored. Therefore, this work demonstrates an application of the slot-die coating technique to print the perovskite active layer of BC PSCs with QIBC electrodes on flexible polymer substrates. The morphology of the obtained perovskite films on QIBC electrodes are investigated and the primary photoelectric parameters of the resulting BC PSCs are measured. The charge carrier recombination processes in the fabricated BC PSCs are investigated and the dominant mechanism for carrier loss in the devices is determined. The findings of the work give an insight into the properties of the slot-die-coated perovskite active layer of BC PSCs and points to exciting new research opportunities in this direction.

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