RESUMEN
Tin-lead (Sn-Pb) perovskite solar cells (PSCs) hold considerable potential for achieving efficiencies near the Shockley-Queisser (S-Q) limit. Notably, the inverted structure stands as the preferred fabrication method for the most efficient Sn-Pb PSCs. In this regard, it is imperative to implement a strategic customization of the hole selective layer to facilitate carrier extraction and refine the quality of perovskite films, which requires effective hole selectivity and favorable interactions with Sn-Pb perovskites. Herein, we propose the development of Co-Self-Assembled Monolayers (Co-SAM) by integrating both [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) and glycine at the buried contacts. The one-step deposition process employed in the fabrication of the Co-SAM ensures uniform coverage, resulting in a homogeneous surface potential. This is attributed to the molecular interactions occurring between 2PACz and glycine in the processing solution. Furthermore, the amine (-NH2) and ammonium (-NH3+) groups in glycine effectively passivate Sn4+ defects at the buried interface of Sn-Pb perovskite films, even under thermal stress. Consequently, the synergistic buried interface regulation of Co-SAM leads to a power conversion efficiency (PCE) of 23.46%, which outperforms devices modified with 2PACz or glycine alone. The Co-SAM-modified Sn-Pb PSC demonstrates enhanced thermal stability, maintaining 88% of its initial PCE under 65 °C thermal stress for 590 h.
RESUMEN
Phenyl-C61-butyric acid methyl ester (PCBM) can be used as a passivation material in perovskite solar cells (PeSCs) in order to reduce the trap site of the perovskite. Here, we show that a thick PCBM layer can form a smoother surface on the SnO2 substrate, improving the grain size and reducing the microstrain of the perovskite. High-temperature annealing treatment of PCBM layer not only increases its solvent resistance to perovskite precursor or antisolvent, but also enhances its molecular alignment, resulting in improved conductivity as an electron transport layer. High-temperature annealed PCBM (HT-PCBM) effectively minimizes trap-assisted nonradiative recombination by reducing trap density in perovskite and improving the electrical properties at the interface between SnO2 and perovskite layers. This HT-PCBM process significantly enhances the performance of the PeSCs, including the open-circuit voltage (VOC) from 0.39 to 0.77 V, fill factor from 52% to 65%, and power conversion efficiency (PCE) from 6.03% to 15.50%, representing substantial improvements compared to devices without PCBM. This PCE is the highest efficiency among conventional (n-i-p) Sn-Pb PeSCs reported to date. Moreover, passivating the trap sites of SnO2 and separating the interface between the Sn-containing perovskite and the substrate effectively have improved the stability of the Sn-Pb perovskite in the n-i-p structure. The optimized best device with HT-PCBM has maintained an efficiency of over 90% for more than 300 h at 85 °C and 5000 h at room temperature in a glovebox atmosphere.