The high-throughput fabrication of PSCs cannot be realized until the costly, low-throughput evaporated metal electrode is replaced by roll-to-roll (R2R) printable (vacuum-free) electrodes. From our understanding, the highest reported power conversion efficiencies (PCEs) for R2R processed PSCs with an evaporated Au electrode and printed back electrode are 13.8% and 4.9%, respectively.[1, 2] In the present work, we introduce a vacuum-free, solvent-free, scalable, and R2R-compatible method to fabricate, and deposit printed electrodes based on electrically conductive pastes. Using this method we avoid potential losses of PSC performance due to solvent migration from the pastes, and additional annealing steps during the electrode deposition. Flexible, R2R-fabricated PSCs with record power conversion efficiencies (PCE) of up to 16.7% were produced by vacuum-free deposition of all active layers, apart from the transparent conductive electrode. This performance compares very favorably with control flexible PSCs comprising an evaporated gold electrode which displayed record PCEs of up to 17.4%. The flexible devices comprising the printed electrode demonstrate outstanding operational and mechanical stability, with negligible loss of PCE after 24 hours of continuous 1-sun illumination and retention of more than 90% of their initial PCE after 3000 cyclic bends. The devices and modules (100 cm2) were completely fabricated in ambient air using readily up-scalable printing and coating technologies.

Furthermore, we have developed a means to deposit the printed electrodes onto rigid, glass-based PSCs to achieve PCEs of over 20% (0.16 cm² active area), only marginally lower than the 20.7% achieved for the control evaporated gold devices. This readily scalable method provides a pathway forward to substantially improve the production throughput as the electrodes can be deposited on potentially hundreds of cells within a matter of minutes using industrially available equipment. In addition, we significantly reduce (almost halve) the total manufacturing cost of the PSCs by removing the time-consuming and expensive gold evaporation process, all while still retaining exceptional photovoltaic performance. This novel electrode deposition method can be readily adapted to demonstrate record-breaking PSCs incorporating low-cost, printed electrodes.