TY - JOUR
T1 - Alternative Organic Spacers for More Efficient Perovskite Solar Cells Containing Ruddlesden-Popper Phases
AU - Xi, Jun
AU - Spanopoulos, Ioannis
AU - Bang, Kijoon
AU - Xu, Jie
AU - Dong, Hua
AU - Yang, Yingguo
AU - Malliakas, Christos D.
AU - Hoffman, Justin M.
AU - Kanatzidis, Mercouri G.
AU - Wu, Zhaoxin
N1 - Funding Information:
This work was supported in part by the National Natural Science Foundation of China (Grants 11574248 and 61505161). China Postdoctoral Science Foundation (Grant 2016M590947), Scientific Research Plan Projects of Shaanxi Education Department (Grant 17JK0700), Natural Science Basic Research Plan in Shaanxi Province of China (Grant 2019JQ-119), and Fundamental Research Funds for the Central Universities (Grant xjj2016031). J.X. and K.B. acknowledge support from the Global Frontier R&D Program of the Center for Multiscale Energy System (Grant 2012M3A6A7054855) by the National Research Foundation under the Ministry of Education, Science and Technology, Korea. The work on perovskite solar cells at Northwestern University was supported by ONR Grant N00014-20-1-2725. This work made use of the IMSERC and EPIC facilities at Northwestern University, which have received support from the SHyNE Resource (NSF ECCS-1542205), the IIN, and Northwestern’s MRSEC program (NSF DMR-1720139), the State of Illinois, and Northwestern University.
PY - 2020/11/18
Y1 - 2020/11/18
N2 - The halide perovskite Ruddlesden-Popper (RP) phases are a homologous layered subclass of solution-processable semiconductors that have aroused great attention, especially for developing long-term solar photovoltaics. They are defined as (A′)2(A)n-1PbnX3n+1 (A′ = spacer cation, A = cage cation, and X = halide anion). The orientation control of low-temperature self-assembled thin films is a fundamental issue associated with the ability to control the charge carrier transport perpendicular to the substrate. Here we report new chemical derivatives designed from a molecular perspective using a novel spacer cation 3-phenyl-2-propenammonium (PPA) with conjugated backbone as a low-temperature strategy to assemble more efficient solar cells. First, we solved and refined the crystal structures of single crystals with the general formula (PPA)2(FA0.5MA0.5)n-1PbnI3n+1 (n = 2 and 3, space group C2) using X-ray diffraction and then used the mixed halide (PPA)2(Cs0.05(FA0.88MA0.12)0.95)n-1Pbn(I0.88Br0.12)3n+1 analogues to achieve more efficient devices. While forming the RP phases, multiple hydrogen bonds between PPA and inorganic octahedra reinforce the layered structure. For films we observe that as the targeted layer thickness index increases from n = 2 to n = 4, a less horizontal preferred orientation of the inorganic layers is progressively realized along with an increased presence of high-n or 3D phases, with an improved flow of free charge carriers and vertical to substrate conductivity. Accordingly, we achieve an efficiency of 14.76% for planar p-i-n solar cells using PPA-RP perovskites, which retain 93.8 ± 0.25% efficiency with encapsulation after 600 h at 85 °C and 85% humidity (ISOS-D-3).
AB - The halide perovskite Ruddlesden-Popper (RP) phases are a homologous layered subclass of solution-processable semiconductors that have aroused great attention, especially for developing long-term solar photovoltaics. They are defined as (A′)2(A)n-1PbnX3n+1 (A′ = spacer cation, A = cage cation, and X = halide anion). The orientation control of low-temperature self-assembled thin films is a fundamental issue associated with the ability to control the charge carrier transport perpendicular to the substrate. Here we report new chemical derivatives designed from a molecular perspective using a novel spacer cation 3-phenyl-2-propenammonium (PPA) with conjugated backbone as a low-temperature strategy to assemble more efficient solar cells. First, we solved and refined the crystal structures of single crystals with the general formula (PPA)2(FA0.5MA0.5)n-1PbnI3n+1 (n = 2 and 3, space group C2) using X-ray diffraction and then used the mixed halide (PPA)2(Cs0.05(FA0.88MA0.12)0.95)n-1Pbn(I0.88Br0.12)3n+1 analogues to achieve more efficient devices. While forming the RP phases, multiple hydrogen bonds between PPA and inorganic octahedra reinforce the layered structure. For films we observe that as the targeted layer thickness index increases from n = 2 to n = 4, a less horizontal preferred orientation of the inorganic layers is progressively realized along with an increased presence of high-n or 3D phases, with an improved flow of free charge carriers and vertical to substrate conductivity. Accordingly, we achieve an efficiency of 14.76% for planar p-i-n solar cells using PPA-RP perovskites, which retain 93.8 ± 0.25% efficiency with encapsulation after 600 h at 85 °C and 85% humidity (ISOS-D-3).
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U2 - 10.1021/jacs.0c09647
DO - 10.1021/jacs.0c09647
M3 - Article
C2 - 33147413
AN - SCOPUS:85096361763
VL - 142
SP - 19705
EP - 19714
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 46
ER -