Function of Porous Carbon Electrode during the Fabrication of Multiporous-Layered-Electrode Perovskite Solar Cells

We demonstrate the effect of sheet conductivity and infiltration using the example of two graphite types, showing that, in general, the graphite type is very important. Amorphous and pyrolytic graphite were applied to carbon electrodes in fully printable carbon-based multiporous-layered-electrode perovskite solar cells (MPLE-PSCs): <glass/F-doped SnO2/compact-TiO2/porous-TiO2+perovskite/porous-ZrO2+perovskite/porous-carbon+perovskite>. The power conversion efficiency (PCE) using amorphous graphite-based carbon (AGC) electrode was only 5.97% due to the low short-circuit photocurrent density (Jsc) value, which was due to the low incident photon-to-current efficiency (IPCE) in the short wavelength region caused by the poor perovskite filling into the porous TiO2-ZrO2 layers. Conversely, using pyrolytic graphite-based carbon (PGC) electrode, Jsc, open-circuit photovoltage (Voc), fill factors (FF), and PCE values of 21.09 mA cm−2, 0.952 V, 0.670, and 13.45%, respectively, were achieved in the champion device. PGC had poorer wettability and a small specific surface area as compared with AGC, but it had better permeability of the perovskite precursor solution into the porous TiO2/ZrO2 layers, and therefore a denser filling and crystallization of the perovskite within the porous TiO2/ZrO2 layers than AGC. It is confirmed that the permeability of the precursor solution depends on the morphology and structure of the graphite employed in the carbon electrode.