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Ambient Blade Coating of Mixed Cation, Mixed Halide Perovskites without Drip: In Situ Investigation and Highly Efficient Solar Cells

Abstract

Perovskite photovoltaics have made extraordinary strides in efficiency and stability thanks to process and formulation developments like the anti-solvent drip and mixed-cation mixed-halide compositions. Solar cell fabrication through low-cost scalable methods, such as blade coating cannot accommodate the anti-solvent drip and needs to be performed in ambient atmosphere. Consequently, their efficiency has lagged behind that of spin-cast devices, fabricated in inert atmosphere and with carefully timed anti-solvent drip to control nucleation and growth. In this study, we demonstrate formamidinium (FA)-dominated mixed-halide mixed-cation perovskite solar cells fabricated by blade coating in ambient air (T = 23 ℃, RH ≈ 50 %) without the benefits of anti-solvent drip or a moisture-free environment. We investigated the solidification process during blade coating of single-cation (FAPbI3) and increasingly complex mixed-cation mixed-halide (FA0.8MA0.15Cs0.05PbI2.55Br0.45, MA is methylammonium) perovskites in situ using time-resolved grazing incidence wide-angle X-ray scattering (GIWAXS). We found that the perovskite precursor composition and the blade coating temperature profoundly influence the crystallization mechanism and whether halide segregation occurs. The inclusion of Br- suppresses the non-perovskite 2H phase, promoting instead PbI2 together with the intermediate 6H phase and 3C phase of FAPbI2.55Br0.45. Addition of Cs+ suppresses these intermediates and promotes the direct crystallization of the perovskite 3C phase FA0.8MA0.15Cs0.05PbI2.55Br0.45 when coating at elevated temperature, unlike when anti-solvent drip is used at room temperature. Through control of ink formulation and coating conditions, we demonstrate blade coated perovskite solar cells with a champion power conversion efficiency (PCE) of 18.20 % as compared with FAPbI3 perovskites, which yield a PCE of 12.35 % in similar conditions without the benefit of anti-solvent drip. This study provides valuable insight into the crystallization pathway of mixed-cation mixed-halide formulations without anti-solvent drip in high-temperature processing conditions that enable the translation of perovskites toward upscalable ambient manufacturing in high throughput conditions.

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Publication details

The article was accepted on 04 Dec 2019 and first published on 04 Dec 2019


Article type: Communication
DOI: 10.1039/C9TA12890E
J. Mater. Chem. A, 2019, Accepted Manuscript

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    Ambient Blade Coating of Mixed Cation, Mixed Halide Perovskites without Drip: In Situ Investigation and Highly Efficient Solar Cells

    M. Tang, Y. Fan, D. Barrit, X. Chang, H. X. Dang, R. Li, K. Wang, D. M. Smilgies, S. Liu, S. De Wolf, T. D. Anthopoulos, K. Zhao and A. Amassian, J. Mater. Chem. A, 2019, Accepted Manuscript , DOI: 10.1039/C9TA12890E

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