Stabilizing Top Interface by Molecular Locking Strategy with Polydentate Chelating Biomaterials toward Efficient and Stable Perovskite Solar Cells in Ambient Air.

The instability of top interface induced by interfacial defects and residual tensile strain hinders the realization of long-term stable n-i-p regular perovskite solar cells (PSCs). Herein, one molecular locking strategy is reported to stabilize top interface by adopting polydentate ligand green biomaterial 2-deoxy-2,2-difluoro-d-erythro-pentafuranous-1-ulose-3,5-dibenzoate (DDPUD) to manipulate the surface and grain boundaries of perovskite films. Both experimental and theoretical evidence collectively uncover that the uncoordinated Pb2+ ions, halide vacancy, and/or I─Pb antisite defects can be effectively healed and locked by firm chemical anchoring on the surface of perovskite films. The ingenious polydentate ligand chelating is translated into reduced interfacial defects, increased carrier lifetimes, released interfacial stress, and enhanced moisture resistance, which should be liable for strengthened top interface stability and inhibited interfacial nonradiative recombination. The universality of the molecular locking strategy is certified by employing different perovskite compositions. The DDPUD modification achieves an enhanced power conversion efficiency (PCE) of 23.17-24.47%, which is one of the highest PCEs ever reported for the devices prepared in ambient air. The unsealed DDPUD-modified devices maintain 98.18% and 88.10% of their initial PCEs after more than 3000 h under a relative humidity of 10-20% and after 1728 h at 65 °C, respectively.

Polydentate Ligand Reinforced Chelating to Stabilize Buried Interface toward High-Performance Perovskite Solar Cells.

The instability of the buried interface poses a serious challenge for commercializing perovskite photovoltaic technology. Herein, we report a polydentate ligand reinforced chelating strategy to strengthen the stability of buried interface by managing interfacial defects and stress. The bis(2,2,2-trifluoroethyl) (methoxycarbonylmethyl)phosphonate (BTP) is employed to manipulate the buried interface. The C=O, P=O and two -CF3 functional groups in BTP synergistically passivate the defects from the surface of SnO2 and the bottom surface of the perovskite layer. Moreover, The BTP modification contributes to mitigated interfacial residual tensile stress, promoted perovskite crystallization, and reduced interfacial energy barrier. The multidentate ligand modulation strategy is appropriate for different perovskite compositions. Due to much reduced nonradiative recombination and heightened interface contact, the device with BTP yields a promising power conversion efficiency (PCE) of 24.63 %, which is one of the highest efficiencies ever reported for devices fabricated in the air environment. The unencapsulated BTP-modified devices degrade to 98.6 % and 84.2 % of their initial PCE values after over 3000 h of aging in the ambient environment and after 1728 h of thermal stress, respectively. This work provides insights into strengthening the stability of the buried interface by engineering multidentate chelating ligand molecules.

1-Adamantanamine Hydrochloride Resists Environmental Corrosion to Obtain Highly Efficient and Stable Perovskite Solar Cells.

Passivating the defective surface of perovskite film is a promising strategy to improve the stability and efficiency of perovskite solar cells (PSCs). Herein, 1-adamantanamine hydrochloride (ATH) is introduced to the upper surface of the perovskite film to heal the defects of the perovskite surface. The best-performance ATH-modified device has a higher efficiency (23.45%) than the champion control device (21.53%). The defects are passivated, interfacial nonradiative recombination is suppressed, and interface stress is released by the ATH deposited on the perovskite film, leading to longer carrier lifetimes and enhancement in open-circuit voltage (VOC) and fill factor (FF) of the PSCs. With obvious improvement, VOC and FF of 1.159 V and 0.796 for the control device are raised to 1.178 V and 0.826 for the ATH-modified device, respectively. Finally, during an operational stability measurement of more than 1000 h, the ATH-treated PSC exhibited better moisture resistance, thermal persistence, and light stability.