Highly Stable O‐Tolylbiguanide‐CsPbI3 Quantum Dots and Light‐Emitting Diodes by Synergistic Supramolecular Passivation

Abstract

AbstractDeveloping effective strategy to passivate surface defects in quantum dots (QDs) is critical to achieving high‐efficiency and long‐life perovskite light‐emitting diodes (LEDs). Here, the supramolecular interaction underpinning of organic‐inorganic components is exploited and a facile method is proposed to generate multiple‐hydrogen‐bonded supramolecular‐perovskite crystal structures on QD surfaces by introducing O‐Tolylbiguanide (O‐Tg) during QD synthesis, enabling bright, conductive, and water‐resistant CsPbI3 QDs. Compared with commonly used oleic acid and oleylamine ligands, the biguanide functional group in O‐Tg not only forms multiple hydrogen bond interactions with lead halide octahedra passivating both bridging‐ and terminal‐halogen ion defects, but also compatibly occupies the A‐site position stabilizing the crystal structure simultaneously. With fewer nonradiative defects and introduced hydrophobic benzene rings preventing eroding of polar molecules, CsPbI3 QDs exhibit remarkable photoluminescence quantum yields of 96%, and their film can be submerged in water for 30 h without degrading. The corresponding LEDs display a high external quantum efficiency (21.2%) and offer superior operational stability with a lifetime (T90) of 25 h at a constant current density as high as 50 mA cm−2.