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Although perovskite solar cells have achieved great development in the device performance, the device stability is still a crucial issue hinder the further development. The ion migration is a main reason for the poor stability of the perovskite solar cells. Here, we use a cross-linking material, polydimethylsiloxane (PDMS) to dope the perovskite layer to improve the operational stability. We systematically studied the effect of curing agent content in PDMS on the device performance and stability. The characterization of perovskite film indicates that PDMS primarily doped in the perovskite layer and as well as enriched at the surface of perovskite film. Doping of PDMS promoted the crystallization of perovskite phase, leading to increase of short circuit density (JSC) and fill factor (FF) of the solar cells. In addition, PDMS doping improved the operational stability of device due to the suppressing the migration of iodide ions during aging. Moreover, the higher content of curing agents used in PDMS, the better stability of the devices. This work indicates PDMS doping the perovskite layer with a suitable content of curing agent can produce a better operational stability of the perovskite solar cells.

n–i–p Type perovskite solar cells generally require air oxidation of the Spiro-OMeTAD layer to achieve high power conversion efficiency (PCE). However, the detailed oxidation mechanism is still not fully understood. In this paper, oxidation of Spiro-OMeTAD was demonstrated via a non-contact electrochemical route using UV-Vis absorption, laser beam induced current (LBIC) imaging and secondary ion mass spectrometry (SIMS) profiling of the Spiro-OMeTAD films. At the cathode, oxygen is reduced to form OH− with the help of H2O, while the anodic reaction is the oxidation of Spiro-OMeTAD to form Spiro-OMeTAD+. Diffusion of Li+ towards the surface of the Ag electrode completes the electrochemical cycle and increases the conductivity of the hole-transporting layer. SIMS analyses of the completed devices demonstrate that the oxidation of Spiro-OMeTAD also leads to migration of Li+ through the perovskite layer into SnO2, which supposedly leads to an increase of the built-in voltage. We verify these results by incorporation of the experimentally measured Li+ concentration into a numerical drift-diffusion simulation, to replicate solar cell J–V-curves. This work provides a new insight into the oxidation of Spiro-OMeTAD in perovskite solar cells, and demonstrates that Li+ migration is involved in the oxidation of Spiro-OMeTAD.