Printable Free-Standing Hybrid Graphene/Dry-Spun Carbon Nanotube Films as Multifunctional Electrodes for Highly Stable Perovskite Solar Cells.

Perovskite solar cells (PSCs) have attracted immense attention owing to their outstanding power conversion efficiency (PCE). However, their counter electrodes are commonly produced by evaporating metals, such as Ag and Au, under high vacuum conditions, which make the PSCs costly, thereby limiting their large-scale production. In this study, a free-standing hybrid graphene/carbon nanotube film was carefully designed to replace noble metal PSC counter electrodes to reduce the cost and increase the stability of PSCs. A highly conductive and stable hybrid carbon thin film can be easily transferred to the various desired substrates by a simple rolling process. The PSCs with hybrid graphene/carbon nanotube films showed a high PCE of 15.36%. Moreover, the devices exhibited excellent stability and could retain 86% of their initial PCE after storage for 500 h in a high-moisture atmosphere (RH 50%). The outstanding stability of PCEs can be attributed to the efficient moisture blocking by the multilayered graphene/carbon nanotube present in the hybrid film. The thin, flexible, and easy-to-synthesize free-standing hybrid graphene/CNT film with high conductivity showed great potential for realizing the low-cost production of highly stable PSCs.