Cyclic Multi-Site Chelation for Efficient and Stable Inverted Perovskite Solar Cells.

Trap-assisted non-radiative recombination losses and moisture-induced degradation significantly impede the development of highly efficient and stable inverted (p-i-n) perovskite solar cells (PSCs), which require high-quality perovskite bulk. In this research, we mitigate these challenges by integrating thermally stable perovskite layers with Lewis base covalent organic frameworks (COFs). The ordered pore structure and surface binding groups of COFs facilitate cyclic, multi-site chelation with undercoordinated lead ions, enhancing the perovskite quality across both its bulk and grain boundaries. This process not only reduces defects but also promotes improved energy alignment through n-type doping at the surface. The inclusion of COF dopants in p-i-n devices achieves power conversion efficiencies (PCEs) of 25.64 % (certified 24.94 %) for a 0.0748-cm2 device and 23.49 % for a 1-cm2 device. Remarkably, these devices retain 81 % of their initial PCE after 978 hours of accelerated aging at 85°C, demonstrating remarkable durability. Additionally, COF-doped devices demonstrate excellent stability under illumination and in moist conditions, even without encapsulation.

Localized Oxidation Embellishing Strategy Enables High-Performance Perovskite Solar Cells.

Perovskite solar cell (pero-SC) has attracted extensive studies as a promising photovoltaic technology, wherein the electron extraction and transfer exhibit pivotal effect to the device performance. The planar SnO2 electron transport layer (ETL) has contributed the recent record power conversion efficiency (PCE) of the pero-SCs, yet still suffers from surface defects of SnO2 nanoparticles which brings energy loss and phase instability. Herein, we report a localized oxidation embellishing (LOE) strategy by applying (NH4 )2 CrO4 on the SnO2 ETL. The LOE strategy builds up plentiful nano-heterojunctions of p-Cr2 O3 /n-SnO2 and the nano-heterojunctions compensate the surface defects and realize benign energy alignment, which reduces surface non-radiative recombination and voltage loss of the pero-SCs. Meanwhile, the decrease of lattice mismatch released the lattice distortion and eliminated tensile stress, contributing to better stability of the devices. The pero-SCs based on α-FAPbI3 with the SnO2 ETL treated by the LOE strategy realized a PCE of 25.72 % (certified as 25.41 %), along with eminent stability performance of T90 >700 h. This work provides a brand-new view for defect modification of SnO2 electron transport layer.