Solution-processed polycrystalline perovskites (PVKs)
have aroused
tremendous interest in the optoelectronic device field. However, the
inherent high-density defects in the polycrystalline hindered achieving
efficient and stable large-area PVK solar cells (PSCs). Although organic
molecules are already employed to passivate PVK defects, they are
insulating by nature, limiting the carrier transport. Here, we design
an assembly of a small molecule (N,N′-di(propanoic acid)-perylene-3,4,9,10-tetracarboxylic diamide,
PDI) via confinement-assisted supramolecular polymerization technology,
which is used as a binder for grain boundaries to simultaneously passivate
defects and promote carrier transport. The synergistic effect allows
the efficiency of all-air processed carbon-based PSCs to reach a decent
power conversion efficiency of 14.17%. Importantly, the as-prepared
supramolecular assembly completely breaks through the insulating nature
of the single molecule, which exists in the long-term defect passivation
of PSCs by organic molecules. It is expected that this finding may
provide novel design ideas to apply the assemblies to improve the
performance of PSCs.