Department of Physics and Astronomy, Wright Center for Photovoltaics Innovation and Commercialization, The University of Toledo, Toledo, OH, 43606, USA.
School of Electronic Science and Engineering, Southeast University, Nanjing, 210096, PR China.
ChemSusChem. 2016 Dec 8;9(23):3288-3297. doi: 10.1002/cssc.201601027. Epub 2016 Oct 26.
Formamidinium lead triiodide (FAPbI ) is considered as an alternative to methylammonium lead triiodide (MAPbI ) because of its lower band gap and better thermal stability. However, owing to the large size of FA cations, it is difficult to synthesize high-quality FAPbI thin films without the formation of an undesirable yellow phase. Smaller sized cations, such as MA and Cs, have been successfully used to suppress the formation of the yellow phase. Whereas FA and MA lead triiodide perovskite solar cells (PVSCs) have achieved power conversion efficiencies (PCEs) higher than 20 %, the PCEs of formamidinium and cesium lead triiodide (FA Cs PbI ) PVSCs have been only approximately 16.5 %. Herein, we report our examination of the main factors limiting the PCEs of (FA Cs PbI ) PVSCs. We find that one of the main limiting factors could be the small grain sizes (≈120 nm), which leads to relatively short carrier lifetimes. We further find that adding a small amount of lead thiocyanate [Pb(SCN) ] to the precursors can enlarge the grain size of (FA Cs PbI ) perovskite thin films and significantly increase carrier lifetimes. As a result, we are able to fabricate (FA Cs PbI ) PVSCs with significantly improved open-circuit voltages and fill factors and, therefore, enhanced PCEs. With an optimal 0.5 mol % Pb(SCN) additive, the average PCE is increased from 16.18±0.50 (13.45±0.78) % to 18.16±0.54 (16.86±0.63) % for planar FA Cs PbI PVSCs if measured under reverse (forward) voltage scans. The champion cell registers a PCE of 19.57 (18.12) % if measured under a reverse (forward) voltage scan, which is comparable to that of the best-performing MA-containing planar FA-based lead halide PVSCs.
甲脒碘化铅(FAPbI )因其带隙较低和热稳定性较好而被认为是碘化甲基铵铅(MAPbI )的替代品。然而,由于 FA 阳离子的尺寸较大,在不形成不理想的黄相的情况下,很难合成高质量的 FAPbI 薄膜。较小尺寸的阳离子,如 MA 和 Cs,已被成功用于抑制黄相的形成。虽然甲脒和 MA 铅卤钙钛矿太阳能电池(PVSCs)的功率转换效率(PCE)已超过 20%,但甲脒和铯碘化铅(FA Cs PbI )PVSCs 的 PCE 仅约为 16.5%。在此,我们报告了对限制(FA Cs PbI )PVSCs PCE 的主要因素的检查。我们发现,一个主要的限制因素可能是较小的晶粒尺寸(≈120nm),这导致相对较短的载流子寿命。我们进一步发现,在前驱体中添加少量的铅硫氰酸盐[Pb(SCN) ]可以增大(FA Cs PbI )钙钛矿薄膜的晶粒尺寸,并显著增加载流子寿命。因此,我们能够制造出(FA Cs PbI )PVSCs,其开路电压和填充因子有显著提高,因此 PCE 得到增强。通过添加最佳的 0.5mol% Pb(SCN)添加剂,平面 FA Cs PbI PVSCs 的平均 PCE 从 16.18±0.50(13.45±0.78)%提高到 18.16±0.54(16.86±0.63)%,如果在反向(正向)电压扫描下进行测量。如果在反向(正向)电压扫描下进行测量,最佳电池的 PCE 为 19.57(18.12)%,与性能最佳的含 MA 的平面 FA 基卤化铅 PVSCs相当。