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Compositional engineering of perovskite materials for high-performance solar cells

Abstract

Of the many materials and methodologies aimed at producing low-cost, efficient photovoltaic cells, inorganic–organic lead halide perovskite materials1,2,3,4,5,6,7,8,9,10,11,12,13,14,15,16,17 appear particularly promising for next-generation solar devices owing to their high power conversion efficiency. The highest efficiencies reported for perovskite solar cells so far have been obtained mainly with methylammonium lead halide materials1,2,3,4,5,6,7,8,9,10. Here we combine the promising—owing to its comparatively narrow bandgap—but relatively unstable formamidinium lead iodide (FAPbI3) with methylammonium lead bromide (MAPbBr3) as the light-harvesting unit in a bilayer solar-cell architecture13. We investigated phase stability, morphology of the perovskite layer, hysteresis in current–voltage characteristics, and overall performance as a function of chemical composition. Our results show that incorporation of MAPbBr3 into FAPbI3 stabilizes the perovskite phase of FAPbI3 and improves the power conversion efficiency of the solar cell to more than 18 per cent under a standard illumination of 100 milliwatts per square centimetre. These findings further emphasize the versatility and performance potential of inorganic–organic lead halide perovskite materials for photovoltaic applications.

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Figure 1: Characterization of materials.
Figure 2: Characterization of materials.
Figure 3: J–V and IPCE characteristics for the best cell obtained in this study.

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Acknowledgements

This work was supported by the Global Research Laboratory (GRL) Program, the Global Frontier R&D Program of the Center for Multiscale Energy System, funded by the National Research Foundation in Korea, and by a grant from the Korea Research Institute of Chemical Technology (KRICT) 2020 Program for Future Technology in South Korea.

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Authors and Affiliations

Authors

Contributions

N.J.J., J.H.N. and S.I.S. conceived the experiments and analysed and interpreted the data. N.J.J., Y.C.K., J.H.N. and J.S. performed the fabrication of devices, device performance measurements and characterization. N.J.J., W.S.Y. and S.R. carried out the synthesis of materials for perovskites, and S.I.S. prepared TiO2 particles and pastes. The manuscript was mainly written and revised by S.I.S. and J.H.N. The project was planned, directed and supervised by S.I.S. All authors discussed the results and commented on the manuscript.

Corresponding author

Correspondence to Sang Il Seok.

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The authors declare no competing financial interests.

Extended data figures and tables

Extended Data Figure 1 In situ XRD spectra (heating from 100 °C to 170 °C) for FAPbI3 yellow powders prepared at room temperature.

Hexagonal non-perovskite FAPbI3 (P63mc) converted into a trigonal perovskite phase (P3m1) near 150 °C. The (−111) diffraction peak for perovskite FAPbI3 at 2θ = 14.3° appeared at a temperature of 150 °C; simultaneously the main peak of non-perovskite FAPbI3 at 11.6° disappeared.

Extended Data Figure 2 XRD spectra of FAPbI3 powders.

The as-prepared yellow FAPbI3 powder shows a non-perovskite phase and is converted to perovskite phase by annealing at 170 °C. The perovskite FAPbI3 black powder returned to the yellow non-perovskite powder after being stored in air for 10 h; the yellow powder reversibly changed to black perovskite phase by re-annealing at 170 °C.

Extended Data Figure 3 XRD spectra of (FAPbI3)1 − x(MAPbBr3)x cells as a function of x.

XRD spectra of solvent-engineering processed (FA1 − xMAx)Pb(I1 − xBrx)3 films on the mesoporous-TiO2/blocking-TiO2/FTO glass substrate after annealing at 100 °C for 10 min. α, α-phase of FAPbI3; #, peaks diffracted from FTO.

Extended Data Figure 4 Photographs of inorganic–organic hybrid halide powders.

Photographs show the colour of the as-prepared MAPbI3, annealed FAPbI3 at 170 °C, FAPbI3, (FAPbI3)1 − x(MAPbI3)x, (FAPbI3)1 − x(FAPbBr3)x, and (FAPbI3)1 − x(MAPbBr3)x powders with x = 0.15 (from left to right). The (FAPbI3)1 − x(MAPbBr3)x powder is the only black powder among the as-prepared FAPbI3-based materials.

Extended Data Figure 5 XRD spectra of the as-prepared powders at room temperature.

XRD spectra of the as-prepared FAPbI3, (FAPbI3)1 − x(MAPbI3)x, (FAPbI3)1 − x(FAPbBr3)x, and (FAPbI3)1 − x(MAPbBr3)x powders with x = 0.15 (from left to right). Only the (FAPbI3)1 − x(MAPbBr3)x powder shows a pure perovskite phase. α, black perovskite-type polymorph; δ, yellow non-perovskite polymorph.

Extended Data Figure 6 Steady-state current measurement.

Steady-state current measured at a maximum power point (0.89 V) and stabilized power output.

Extended Data Figure 7 Photovoltaic performance.

a, J–V curves measured by forward and reverse bias sweep and their averaged curve for cell using the (FAPbI3)0.85(MAPbBr3)0.15 perovskite active layer and 80-nm-thick mesoporous-TiO2 layer. η, PCE. b, Steady-state current measured at a maximum power point (0.92 V)and stabilized power output.

Extended Data Figure 8 Independent certification from Newport Corporation, confirming a PCE of 17.9%.

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Jeon, N., Noh, J., Yang, W. et al. Compositional engineering of perovskite materials for high-performance solar cells. Nature 517, 476–480 (2015). https://doi.org/10.1038/nature14133

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