Macroscale and Nanoscale Morphology Evolution during in Situ Spray Coating of Titania Films for Perovskite Solar Cells

Mesoporous titania is a cheap and widely used material for photovoltaic applications. To enable a large-scale fabrication and a controllable pore size, we combined a block copolymer-assisted sol–gel route with spray coating to fabricate titania films, in which the block copolymer polystyrene-block-poly(ethylene oxide) (PS-b-PEO) is used as a structure-directing template. Both the macroscale and nanoscale are studied. The kinetics and thermodynamics of the spray deposition processes are simulated on a macroscale, which shows a good agreement with the large-scale morphology of the spray-coated films obtained in practice. On the nanoscale, the structure evolution of the titania films is probed with in situ grazing incidence small-angle X-ray scattering (GISAXS) during the spray process. The changes of the PS domain size depend not only on micellization but also on solvent evaporation during the spray coating. Perovskite (CH3NH3PbI3) solar cells (PSCs) based on sprayed titania film are fabricated, which showcases the suitability of spray-deposited titania films for PSCs.