Ethylenediamine (EDA, amine-based
Lewis base) was utilized as a
base catalyst in the synthesis of nickel oxide (NiO
x
) to regulate the coordination properties of metal ions (Lewis
acid). The effect of the EDA chelating agent on the hole transporting
properties of NiO
x
was determined according
to crystal field theory. The particle size in the NiO
x
thin film changed according to the EDA molar ratio,
which influenced the electrical properties and affinity with the photoactive
layer. Excellent electrical conductivity and improved crystallinity
of the perovskite layer were confirmed via a conductive atomic force
microscope (C-AFM), X-ray diffraction (XRD), and field emission scanning
electron microscope (FE-SEM) analyses at the optimal EDA ratio in
NiO
x
. In particular, UPS (reduced energy
band offset) and charge dynamics data demonstrate the enhanced short
circuit current, fill factor, and efficiency of the perovskite solar
cells. Comprehensively, this study supports the role and effect of
the EDA chelating agent in NiO
x
for next-generation
solar cells. Moreover, it provides insight into the understanding
and potential of various sol–gel materials synthesized based
on crystal field theory.