Fully printed perovskite solar cells are demonstrated with slot-die coating, a scalable printing method. A sequential slot-die coating process is developed to produce efficient perovskite solar cells and to be used in a large-scale roll-to-roll printing process. All layers excluding the electrodes are printed and devices demonstrate up to 11.96% power conversion efficiency. It is also demonstrated that the new process can be used in roll-to-roll production.

Driven by recent improvements in efficiency and stability of perovskite solar cells (PSCs), upscaling of PSCs has come to be regarded as the next step. Specifically, a high-throughput, low-cost roll-to-roll (R2R) processes would be a breakthrough to realize the commercialization of PSCs, with uniform formation of precursor wet film and complete conversion to perovskite phase via R2R-compatible processes necessary to accomplish this goal. Herein, we demonstrate the pilot-scale, fully R2R manufacturing of all the layers except for electrodes in PSCs. Tert-butyl alcohol (tBuOH) is introduced as an eco-friendly antisolvent with a wide processing window. Highly crystalline, uniform formamidinium (FA)-based perovskite formation via tBuOH:EA bathing was confirmed by achieving high power conversion efficiencies (PCEs) of 23.5% for glass-based spin-coated PSCs, and 19.1% for gravure-printed flexible PSCs. As an extended work, R2R gravure-printing and tBuOH:EA bathing resulted in the highest PCE reported for R2R-processed PSCs, 16.7% for PSCs with R2R-processed SnO2/FA-perovskite, and 13.8% for fully R2R-produced PSCs.

A 3D printer based slot‐die coater is developed as a lab‐to‐fab translation tool for solution‐processed solar cells. The modified 3D printer is used to develop the printing process for potential use in large scale roll‐to‐roll production. Fabrication of a 47.3 cm2 organic solar cell module with 4.56% efficiency and printed perovskite solar cells with 11.6% efficiency are demonstrated.