Hybrid halide 2D perovskites deserve special attention because they exhibit superior environmental stability compared with their 3D analogs. The closer interlayer distance discovered in 2D Dion–Jacobson (DJ) type of halide perovskites relative to 2D Ruddlesden–Popper (RP) perovskites implies better carrier charge transport and superior performance in solar cells. Here, the structure and properties of 2D DJ perovskites employing 3‐(aminomethyl)piperidinium (3AMP2+) as the spacing cation and a mixture of methylammonium (MA+) and formamidinium (FA+) cations in the perovskite cages are presented. Using single‐crystal X‐ray crystallography, it is found that the mixed‐cation (3AMP)(MA0.75FA0.25)3Pb4I13perovskite has a narrower bandgap, less distorted inorganic framework, and larger PbIPb angles than the single‐cation (3AMP)(MA)3Pb4I13. Furthermore, the (3AMP)(MA0.75FA0.25)3Pb4I13films made by a solvent‐engineering method with a small amount of hydriodic acid have a much better film morphology and crystalline quality and more preferred perpendicular orientation. As a result, the (3AMP)(MA0.75FA0.25)3Pb4I13‐based solar cells exhibit a champion power conversion efficiency of 12.04% with a high fill factor of 81.04% and a 50% average efficiency improvement compared to the pristine (3AMP)(MA)3Pb4I13cells. Most importantly, the 2D DJ 3AMP‐based perovskite films and devices show better air and light stability than the 2D RP butylammonium‐based perovskites and their 3D analogs.
Metal‐halide perovskites have become appealing materials for optoelectronic devices. While the fast advancing stretchable/wearable devices require stability, flexibility and scalability, current perovskites suffer from ambient‐environmental instability and incompatible mechanical properties. Recently perovskite−polymer composites have shown improved in‐air stability with the protection of polymers. However, their stability remains unsatisfactory in water or high‐humidity environment. These methods also suffer from limited processability with low yield (2D film or beads) and high fabrication cost (high temperature, air/moisture‐free conditions), thereby limiting their device integration and broader applications. Herein, by combining facile photo‐polymerization with room‐temperature in‐situ perovskite reprecipitation at low energy cost, a one‐step scalable method is developed to produce freestanding highly‐stable luminescent organogels, within which CH3NH3PbBr3nanoparticles are homogeneously distributed. The perovskite‐organogels present a record‐high stability at different pH and temperatures, maintaining their high quantum yields for > 110 days immersing in water. This paradigm is universally applicable to broad choices of polymers, hence casting these emerging luminescent materials to a wide range of mechanical properties tunable from rigid to elastic. With intrinsically ultra‐stretchable photoluminescent organogels, flexible phosphorous layers were demonstrated with > 950% elongation. Rigid perovskite gels, on the other hand, permitted the deployment of 3D‐printing technology to fabricate arbitrary 2D/3D luminescent architectures.
more » « less- NSF-PAR ID:
- 10460173
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 31
- Issue:
- 37
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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