Water-Soluble Triazolium Ionic-Liquid-Induced Surface Self-Assembly to Enhance the Stability and Efficiency of Perovskite Solar Cells

Despite being a promising candidate for next-generation photovoltaics, perovskite solar cells (PSCs) exhibit limited stability that hinders their practical application. In order to improve the humidity stability of PSCs, herein, a series of ionic liquids (ILs) “1-alkyl-4-amino-1,2,4-triazolium” (termed as RATZ; R represents alkyl chain, and ATZ represents 4-amino-1,2,4-triazolium) as cations are designed and used as additives in methylammonium lead iodide (MAPbI ₃ ) perovskite precursor solution, obtaining triazolium ILs-modified PSCs for the first time (termed as MA/RATZ PSCs). As opposed to from traditional methods that seek to improve the stability of PSCs by functionalizing perovskite film with hydrophobic molecules, humidity-stable perovskite films are prepared by exploiting the self-assembled monolayer (SAM) formation of water-soluble triazolium ILs on a hydrophilic perovskite surface. The mechanism is validated by experimental and theoretical calculation. This strategy means that the MA/RATZ devices exhibit good humidity stability, maintaining around 80% initial efficiency for 3500 h under 40 ± 5% relative humidity. Meanwhile, the MA/RATZ PSCs exhibit enhanced thermal stability and photostability. Tuning the molecule structure of the ILs additives achieves a maximum power conversion efficiency (PCE) of 20.03%. This work demonstrates the potential of using triazolium ILs as additives and SAM and molecular design to achieve high performance PSCs.