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Forming a Metal-Free Oxidatively Coupled Agent, Bicarbazole, as a Defect Passivation for HTM and an Interfacial Layer in a p–i–n Perovskite Solar Cell Exhibits Nearly 20% Efficiency
journal contribution
posted on 2019-10-17, 15:05 authored by Sudhakar Maddala, Chung-Lin Chung, Shin-Yu Wang, Kalidass Kollimalayan, Hsiang-Lin Hsu, Parthasarathy Venkatakrishnan, Chih-Ping Chen, Yuan Jay ChangIn
this study, we synthesized three simple and inexpensive (34–120
USD/g) 3,3′-bicarbazole-based hole transporting materials (BC-HTMs; NP-BC, NBP-BC and PNP-BC) through a metal-free oxidative coupling, in excellent
yields (≥95%). These bicarbazoles contain phenylene or biphenylene
substituents on the carbazole N atom, with extended π-conjugation
achieved through phenylene units at the 6,6′-positions of the
bicarbazole. When using NBP-BC as a dopant-free HTM in
a p–i–n perovskite solar cell (PSC), we achieved a power
conversion efficiency (PCEs) of 12.22 ± 0.54% under AM 1.5G conditions
(100 mW cm–2); this PCE was comparable to that obtained
when using PEDOT:PSS as the HTM (11.23 ± 1.02%). BC-HTMs showed the large grain size (μm) of perovskite than PEDOT:PSS-based,
due to defect passivation on indium tin oxide (ITO) substrate and
good hydrophobicity. Furthermore, we realized highly efficient and
stable PSCs when using the p–i–n device structure ITO/NiOx/NP-BC/perovskite/PC61BM/BCP/Ag. The bifacial defect passivation effect of the interfacial
layer improved the grain size of the perovskite layer and also enhanced
the performance; the best performance of the NiOx/NP-BC device was characterized by a short-circuit
current density (Jsc) of 22.38 mA cm–2, an open-circuit voltage (Voc) of 1.09 V, and a fill factor (FF) of 79.9%, corresponding
to an overall PCE of almost 20%. This device structure has competitive
potential because its performance is comparable to that of the record-high-efficiency
PSCs. Under an Ar atmosphere, the PCE of the NiOx/NP-BC PSC device decayed by only 4.55% after
168 h; it retained 90.80% of its original PCE after 1000 h. A morphological
study revealed that the films of the BC-HTMs were indeed
smooth and hydrophobic and that the perovskite films spin-coated upon
them were uniform and featured large grains (micrometer scale). Time-resolved
photoluminescence (TRPL) spectra of the perovskite films suggested
that the hole extraction capabilities of the NiOx/BC-HTMs were better than that of the bare NiOx. The superior film morphologies of the NiOx/BC-HTMs were responsible for
the performances of their devices being comparable to those of bare
NiOx-based PSCs.