Using Soft Polymer Template Engineering of Mesoporous TiO₂ Scaffolds to Increase Perovskite Grain Size and Solar Cell...

The mesoporous (meso)-TiO₂ layer is a key component of high-efficiency perovskite solar cells (PSCs). Herein, pore size controllable meso-TiO₂ layers are prepared using spin coating of commercial TiO₂ nanoparticle (NP) paste with added soft polymer templates (SPT) followed by removal of the SPT at 500 °C. The SPTs consist of swollen crosslinked polymer colloids (microgels, MGs) or a commercial linear polymer (denoted as LIN). The MGs and LIN were comprised of the same polymer, which was poly(N-isopropylacrylamide) (PNIPAm). Large (L-MG) and small (S-MG) MG SPTs were employed to study the effect of the template size. The SPT approach enabled pore size engineering in one deposition step. The SPT/TiO₂ nanoparticle films had pore sizes > 100 nm, whereas the average pore size was 37 nm for the control meso-TiO₂ scaffold. The largest pore sizes were obtained using L-MG. SPT engineering increased the perovskite grain size in the same order as the SPT sizes: LIN < S-MG < L-MG and these grain sizes were larger than those obtained using the control. The power conversion efficiencies (PCEs) of the SPT/TiO₂ devices were ∼20% higher than that for the control meso-TiO₂ device and the PCE of the champion S-MG device was 18.8%. The PCE improvement is due to the increased grain size and more effective light harvesting of the SPT devices. The increased grain size was also responsible for the improved stability of the SPT/TiO₂ devices. The SPT method used here is simple, scalable, and versatile and should also apply to other PSCs.