Anchoring Fullerene onto Perovskite Film via Grafting Pyridine toward Enhanced Electron Transport in High-Efficiency Solar Cells

Fullerene derivatives have been popularly applied as electron transport layers (ETLs) of inverted (p–i–n) planar heterojunction perovskite solar cells (iPSCs) due to their strong electron-accepting abilities, and so far, [6,6]-phenyl-C 61 -butyric acid methyl ester (PCBM) has been the most commonly used ETL, which suffers, however, from high cost due to the complicated synthetic route. Herein, novel pyridine-functionalized fullerene derivatives (abbreviated as C 60 -Py) were synthesized facilely via a one-step 1,3-dipolar cycloaddition reaction and applied as ETLs superior to PCBM in iPSC devices. Three pyridine-functionalized fullerene derivatives with different alkyl groups, including methyl, n -butyl, and n -hexyl, grafted onto the pyrrolidine moiety (abbreviated as C 60 -MPy, C 60 -BPy, and C 60 -HPy, respectively) were synthesized. According to cyclic voltammogram study, the chain length of the N -alkyl group has negligible influence on the molecular energy level of C 60 -Py. However, the ETL performance of C 60 -Py is sensitively dependent on the chain length of the N -alkyl group, with C 60 -BPy exhibiting the highest power conversion efficiency (PCE) of 16.83%, which surpasses that based on PCBM ETL (15.87%). The PCE enhancement of C 60 -BPy device is attributed to the coordination interactions between the pyridine moiety with the Pb 2+ ion of CH 3 NH 3 PbI 3 perovskite, which anchor C 60 -BPy onto perovskite film and reinforce the passivation of the trap state within the CH 3 NH 3 PbI 3 perovskite film and suppress the nonradiative electron–hole recombinations, leading to enhanced electron transport reflected by the increase of short-circuit current density ( J sc ). The ambient stability of C 60 -HPy-based device is much better than that based on PCBM ETL since its long N -alkyl group can function as a superior encapsulating layer protecting the CH 3 NH 3 PbI 3 layer from contact with the ambient moisture.