Multiple Dynamic Hydrogen Bonding Networks Boost the Mechanical Stability of Flexible Perovskite Solar Cells

Abstract Flexible perovskite solar cells often experience constant or cyclic bending during their service life. Catastrophic failure of devices may occur due to the crack of polycrystalline perovskite films and delamination at the perovskite and the substrate interfaces, posing a significant stability concern. Here, a multiple dynamic hydrogen bonding polymer network is developed to enhance the mechanical strength of flexible perovskite solar cells in two ways. The main chain of poly(acrylic acid) decreases the mismatch of the coefficient of thermal expansion between the perovskite and the substrate by 16.7% through its flexibility and spatial occupation. The dopamine branch chains provide multiple dynamic hydrogen bonding sites, which contribute to increased energy dissipation upon stress deformation and reduce Young's modulus of perovskite by 54.3%. The inverted flexible perovskite solar cells achieve a champion power conversion efficiency of 23.02% and retain 81.3% of the initial PCE over 2000 h under continuous 1‐sun equivalent illumination. Moreover, devices show excellent mechanical stability by remaining 90.2% of the original value after 5000 bending cycles.