Abstract
Two-dimensional (2D) and three-dimensional (3D) perovskite heterostructures have played a key role in advancing the performance of perovskite solar cells1,2. However, the migration of cations between 2D and 3D layers results in the disruption of octahedral networks, leading to degradation in performance over time3,4. We hypothesized that perovskitoids, with robust organic–inorganic networks enabled by edge- and face-sharing, could impede ion migration. We explored a set of perovskitoids of varying dimensionality and found that cation migration within perovskitoid–perovskite heterostructures was suppressed compared with the 2D–3D perovskite case. Increasing the dimensionality of perovskitoids improves charge transport when they are interfaced with 3D perovskite surfaces—this is the result of enhanced octahedral connectivity and out-of-plane orientation. The 2D perovskitoid (A6BfP)8Pb7I22 (A6BfP: N-aminohexyl-benz[f]-phthalimide) provides efficient passivation of perovskite surfaces and enables uniform large-area perovskite films. Devices based on perovskitoid–perovskite heterostructures achieve a certified quasi-steady-state power conversion efficiency of 24.6% for centimetre-area perovskite solar cells. We removed the fragile hole transport layers and showed stable operation of the underlying perovskitoid–perovskite heterostructure at 85 °C for 1,250 h for encapsulated large-area devices in ambient air.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 359-364 |
| Number of pages | 6 |
| Journal | Nature |
| Volume | 633 |
| Issue number | 8029 |
| DOIs | |
| State | Published - Sep 12 2024 |
Funding
This work is partially supported by award 70NANB19H005 from the US Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD). M.G.K. was supported by DOE BES grant no. DE-SC0024422 (fundamental studies on metal halides) and T.J.M. by ONR award no. N00014-20-1-2116. This work made use of the SPID, EPIC, Keck-II and NUFAB facilities of Northwestern University\u2019s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the International Institute of Nanotechnology, Northwestern University and Northwestern\u2019s MRSEC programs (NSF DMR-1720139, NSF DMR-2308691). A.S.R.B. acknowledges support from King Abdullah University of Science and Technology (KAUST) through the Ibn Rushd Postdoctoral Fellowship Award.
ASJC Scopus subject areas
- General
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CCDC 2362696: Experimental Crystal Structure Determination
Liu, C. (Contributor), Yang, Y. (Contributor), Chen, H. (Contributor), Spanopoulos, I. (Contributor), Bati, A. S. R. (Contributor), Gilley, I. W. (Contributor), Chen, J. (Contributor), Maxwell, A. (Contributor), Vishal, B. (Contributor), Reynolds, R. P. (Contributor), Wiggins, T. E. (Contributor), Wang, Z. (Contributor), Huang, C. (Contributor), Fletcher, J. (Contributor), Liu, Y. (Contributor), Chen, L. X. (Contributor), De Wolf, S. (Contributor), Chen, B. (Contributor), Zheng, D. (Contributor), Facchetti, A. (Contributor) & Kanatzidis, M. G. (Contributor), Cambridge Crystallographic Data Centre, 2024
DOI: 10.5517/ccdc.csd.cc2k9l0h, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2k9l0h&sid=DataCite
Dataset
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CCDC 2362701: Experimental Crystal Structure Determination
Liu, C. (Contributor), Yang, Y. (Contributor), Chen, H. (Contributor), Spanopoulos, I. (Contributor), Bati, A. S. R. (Contributor), Gilley, I. W. (Contributor), Chen, J. (Contributor), Maxwell, A. (Contributor), Vishal, B. (Contributor), Reynolds, R. P. (Contributor), Wiggins, T. E. (Contributor), Wang, Z. (Contributor), Huang, C. (Contributor), Fletcher, J. (Contributor), Liu, Y. (Contributor), Chen, L. X. (Contributor), De Wolf, S. (Contributor), Chen, B. (Contributor), Zheng, D. (Contributor), Facchetti, A. (Contributor) & Kanatzidis, M. G. (Contributor), Cambridge Crystallographic Data Centre, 2024
DOI: 10.5517/ccdc.csd.cc2k9l5n, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2k9l5n&sid=DataCite
Dataset
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CCDC 2362702: Experimental Crystal Structure Determination
Liu, C. (Contributor), Yang, Y. (Contributor), Chen, H. (Contributor), Spanopoulos, I. (Contributor), Bati, A. S. R. (Contributor), Gilley, I. W. (Contributor), Chen, J. (Contributor), Maxwell, A. (Contributor), Vishal, B. (Contributor), Reynolds, R. P. (Contributor), Wiggins, T. E. (Contributor), Wang, Z. (Contributor), Huang, C. (Contributor), Fletcher, J. (Contributor), Liu, Y. (Contributor), Chen, L. X. (Contributor), De Wolf, S. (Contributor), Chen, B. (Contributor), Zheng, D. (Contributor), Facchetti, A. (Contributor) & Kanatzidis, M. G. (Contributor), Cambridge Crystallographic Data Centre, 2024
DOI: 10.5517/ccdc.csd.cc2k9l6p, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2k9l6p&sid=DataCite
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