Improved performance of hole-transporting
layer-free perovskite solar cells by using graphene
oxide sheets as the nucleation centers
Xue Sun,
ab
Tong Lin,
ab
Qiaogang Song,
ab
Yue Fu,
ab
Ye Wang,
ab
Fangming Jin,
a
Haifeng Zhao,
a
Wenlian Li,
a
Zisheng Su
*
a
and Bei Chu
a
Graphene oxide sheets (GOSs) are introduced between indium tin oxide (ITO) and CH
3
NH
3
PbI
3
in inverted
hole-transport layer-free planar heterojunction perovskite solar cells. The concentration of the GOSs is
extremely low and they are sporadically covered on the ITO substrates. Combined with the high
resistance of these GOSs, they cannot be regarded as an interface layer. However, the GOSs can act as
the nucleation sites in the crystal growth process of CH
3
NH
3
PbI
3
films, which results in dramatically
improved morphology and crystallization of the CH
3
NH
3
PbI
3
films. As a result, the performance of the
devices is significantly improved as compared with the reference device. The optimized device shows
a power conversion efficiency of 6.62%, which is about 40% higher than the reference devices. This
improvement is attributed to the increased charge carrier transporting property and reduced charge
carrier recombination in the CH
3
NH
3
PbI
3
films.
Introduction
Lead-halide perovskite is used as a light absorber and holds
great promise in the eld of efficient and low-cost optoelec-
tronic materials, owing to its extraordinary photonic and elec-
tronic properties. Perovskite solar cells (PSCs) have made
impressive progress with power conversion efficiencies (PCEs)
evolving from 3.8% to a certied 22.1% within just 8 years, and
there is still room for growth.
1–4
To boost the PCE, extensive
research has been devoted to PSC devices, such as improving
charge collection and transport efficiency, optimizing cell
structure, and enhancing the quality of each layer.
5–8
Perovskite
solar cells have two types of cell structures: planar hetero-
junction and mesoscopic structure. Most of efficient meso-
scopic PSCs employed meso-superstructure or condensed metal
oxides such as TiO
2
and Al
2
O
3
, and required high-temperature
(500
C) during the high-quality metal oxides produce pro-
cessing, which is not suitable for fabricating on exible plastic
substrates.
4,9–11
Relative to mesoporous PSCs, planar hetero-
junction devices have attracted much attention because of their
simple structures and preparation process. Unfortunately,
typical organic hole transport layers (HTLs) such as 2,2
0
,7,7
0
-
tetrakis(N,N-di-p-methoxy phenylamine)-9,9-spirobi-uorene
(spiro-OMeTAD) and poly(3,4-ethylene dioxythiophene):poly(s-
tyrene sulfonate) (PEDOT:PSS) are expensive and may result in
instability problems under ambient air.
12
To overcome these
disadvantages, researches on simplied structure like HTL-free
have been put forward. Chen and co-workers fabricated
inverted-structured HTL-free PSCs on exible polyethylene
terephthalate substrates, and a maximum PCE of 9.7% was
obtained. At the same time, the structure of indium tin oxide
(ITO)/CH
3
NH
3
PbI
3
/phenyl-C
61
-butyric acid methyl ester/Al
without HTL achieved a PCE of 12.5%.
13
Ye et al. spin-coated
the hybrid precursor solution with both CuSCN and perov-
skite, and the device of ITO/MAPbI
3x
Cl
x
(CuSCN)/C
60
/
bathocuproine/Ag without HTL layer signicantly accelerated
hole transfer from the perovskite layer to ITO. The device
reached a maximum PCE of 18.1%.
14
Perovskite materials
always exhibit high charge mobility, and therefore they are
possible to be used as both absorb layer and HTL in order to
achieve simple and low-cost HTL-free PSCs.
15
The interfacial energy structures and contact between the
functional layers can directly affect the charge collection and
extraction. Along with appropriate charge transport materials, it
is vitally important for PSCs to have a light absorb layer with
high crystallization and surface coverage. Many methods aimed
to improve the lm quality have been used, such as including
additives into precursor, optimizing the lm-fabrication meth-
odology, improving composition, and perfecting the lm-
fabrication methodology.
16
Liang et al. introduced 1,8-diio-
dooctane into perovskite precursor solution and effectively
controlled the rate of perovskite crystallization.
17
The growth of
perovskite layer can also be manipulated by the insert of bottom
nanoparticles
18,19
and organic layers.
20
a
State Key Laboratory of Luminescence and Applications, Changchun Institute of
Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun
130033, P. R. China. E-mail: suzs@ciomp.ac.cn; chub@ciomp.ac.cn
b
University of Chinese Academy of Sciences, Beijing, 100039, P. R. China
Cite this: RSC Adv.,2017,7, 45320
Received 6th August 2017
Accepted 15th September 2017
DOI: 10.1039/c7ra08680f
rsc.li/rsc-advances
45320 | RSC Adv.,2017,7, 45320–45326 This journal is © The Royal Society of Chemistry 2017
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