Additive and antisolvent engineering strategies are outstandingly
efficient in enhancing perovskite quality, photovoltaic performance,
and stability of perovskite solar cells (PSCs). In this work, an effective
approach is applied by coupling the antisolvent mixture and multi-functional
additive procedures, which is recognized as antisolvent additive engineering
(AAE). The graphene quantum dots functionalized with amide (AGQDs),
which consists of carbonyl, amine, and long hydrophobic alkyl chain
functional groups, are added to the antisolvent mixture of toluene
(T) and hexane (H) as an efficient additive to form the CH3NH3PbI3 (MAPI):AGQDs graded heterojunction
structure. A broad range of analytical techniques, including scanning
electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy,
space charge limited current, UV–visible spectroscopy, external
quantum efficiency, and time-of-flight secondary ion mass spectrometry,
are used to investigate the effect of AAE treatment with AGQDs on
the quality of perovskite film and performance of the PSCs. Importantly,
not only a uniform and dense perovskite film with hydrophobic property
is obtained but also defects on the perovskite surface are significantly
passivated by the interaction between AGQDs and uncoordinated Pb2+. As a result, an enhanced power conversion efficiency (PCE)
of 19.10% is achieved for the champion PSCs treated with AGQD additive,
compared to the PCE of 16.00% for untreated reference PSCs. In addition,
the high-efficiency PSCs based on AGQDs show high stability and maintain
89% of their initial PCE after 960 h in ambient conditions.