Interface Chelation Induced by Pyridine-Based Polymer for Efficient and Durable Air-Processed Perovskite Solar Cells

Angew Chem Int Ed Engl. 2022 Jan 21;61(4):e202112673. doi: 10.1002/anie.202112673. Epub 2021 Dec 10.

Abstract

Polymer doping is a significant approach to precisely control nucleation and crystal growth of perovskites and enhance electronic quality in perovskite solar cells (PSC) prepared in air. Here, a brand-new self-healing polysiloxane (SHP) with dynamic 2,6-pyridinedicarboxamide (PDCA) coordination units and plenty of hydrogen bonds was designed and incorporated into perovskite films. PDCA units, showing strong intermolecular Pb2+ -Namido , I- -Npyridyl , and Pb2+ -Oamido coordination interactions, were expected to enhance crystallinity and passivate the grain boundary. In addition, abundant hydrogen bonds in SHP afforded the self-healing of cracks at grain boundaries for fatigue PSCs. Significantly, the doped device demonstrated a champion efficiency of 19.50 % with inconspicuous hysteresis, almost rivaling those achieved in control atmosphere. This strategy of heterocyclic-based macromolecular doping in PSCs will pave a way for realizing efficient and durable crystalline semiconductors.

Keywords: chelation; grain boundaries; pyridinedicarboxamide; self-healing polydimethylsiloxane; stretchability.