Unraveling the Chemical Nature of the 3D “Hollow” Hybrid Halide Perovskites
Abstract
The newly introduced class of 3D halide perovskites, termed “hollow” perovskites, has been recently demonstrated as light absorbing semiconductor materials for fabricating lead-free perovskite solar cells with enhanced efficiency and superior stability. Hollow perovskites derive from three-dimensional (3D) AMX3 perovskites (A = methylammonium (MA), formamidinium (FA); M = Sn, Pb; X = Cl, Br, I), where small molecules such as ethylenediammonium cations (en) can be incorporated as the dication without altering the structure dimensionality. In this article, we present in this work the inherent structural properties of the hollow perovskites and expand this class of materials to the Pb-based analogues. Through a combination of physical and spectroscopic methods (XRD, gas pycnometry, 1H NMR, TGA, SEM/EDX), we have assigned the general formula (A)1–x(en)x(M)1–0.7x(X)3–0.4x to the hollow perovskites. The incorporation of en in the 3D perovskite structure leads to massive M and X vacancies in the 3D [MX3] framework, thus the term hollow. The resulting materials are semiconductors with significantly blue-shifted direct band gaps from 1.25 to 1.51 eV for Sn-based perovskites and from 1.53 to 2.1 eV for the Pb-based analogues. The increased structural disorder and hollow nature were validated by single crystal X-ray diffraction analysis as well as pair distributionmore »
- Authors:
-
- Northwestern Univ., Evanston, IL (United States)
- Univ. of California, Santa Barbara, CA (United States)
- Publication Date:
- Research Org.:
- Univ. of California, Santa Barbara, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1599736
- Grant/Contract Number:
- SC0012541; AC02-06CH11357; ECCS-1542205; DMR-1720139
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 17; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Spanopoulos, Ioannis, Ke, Weijun, Stoumpos, Constantinos C., Schueller, Emily C., Kontsevoi, Oleg Y., Seshadri, Ram, and Kanatzidis, Mercouri G. Unraveling the Chemical Nature of the 3D “Hollow” Hybrid Halide Perovskites. United States: N. p., 2018.
Web. doi:10.1021/jacs.8b01034.
Spanopoulos, Ioannis, Ke, Weijun, Stoumpos, Constantinos C., Schueller, Emily C., Kontsevoi, Oleg Y., Seshadri, Ram, & Kanatzidis, Mercouri G. Unraveling the Chemical Nature of the 3D “Hollow” Hybrid Halide Perovskites. United States. https://doi.org/10.1021/jacs.8b01034
Spanopoulos, Ioannis, Ke, Weijun, Stoumpos, Constantinos C., Schueller, Emily C., Kontsevoi, Oleg Y., Seshadri, Ram, and Kanatzidis, Mercouri G. Wed .
"Unraveling the Chemical Nature of the 3D “Hollow” Hybrid Halide Perovskites". United States. https://doi.org/10.1021/jacs.8b01034. https://www.osti.gov/servlets/purl/1599736.
@article{osti_1599736,
title = {Unraveling the Chemical Nature of the 3D “Hollow” Hybrid Halide Perovskites},
author = {Spanopoulos, Ioannis and Ke, Weijun and Stoumpos, Constantinos C. and Schueller, Emily C. and Kontsevoi, Oleg Y. and Seshadri, Ram and Kanatzidis, Mercouri G.},
abstractNote = {The newly introduced class of 3D halide perovskites, termed “hollow” perovskites, has been recently demonstrated as light absorbing semiconductor materials for fabricating lead-free perovskite solar cells with enhanced efficiency and superior stability. Hollow perovskites derive from three-dimensional (3D) AMX3 perovskites (A = methylammonium (MA), formamidinium (FA); M = Sn, Pb; X = Cl, Br, I), where small molecules such as ethylenediammonium cations (en) can be incorporated as the dication without altering the structure dimensionality. In this article, we present in this work the inherent structural properties of the hollow perovskites and expand this class of materials to the Pb-based analogues. Through a combination of physical and spectroscopic methods (XRD, gas pycnometry, 1H NMR, TGA, SEM/EDX), we have assigned the general formula (A)1–x(en)x(M)1–0.7x(X)3–0.4x to the hollow perovskites. The incorporation of en in the 3D perovskite structure leads to massive M and X vacancies in the 3D [MX3] framework, thus the term hollow. The resulting materials are semiconductors with significantly blue-shifted direct band gaps from 1.25 to 1.51 eV for Sn-based perovskites and from 1.53 to 2.1 eV for the Pb-based analogues. The increased structural disorder and hollow nature were validated by single crystal X-ray diffraction analysis as well as pair distribution function (PDF) analysis. Density functional theory (DFT) calculations support the experimental trends and suggest that the observed widening of the band gap is attributed to the massive M and X vacancies, which create a less connected 3D hollow structure. The resulting materials have superior air stability, where in the case of Sn-based hollow perovskites it exceeds two orders of temporal magnitude compared to the conventional full perovskites of MASnI3 and FASnI3. Lastly, the hollow perovskite compounds pose as a new platform of promising light absorbers that can be utilized in single junction or tandem solar cells.},
doi = {10.1021/jacs.8b01034},
journal = {Journal of the American Chemical Society},
number = 17,
volume = 140,
place = {United States},
year = {Wed Apr 04 00:00:00 EDT 2018},
month = {Wed Apr 04 00:00:00 EDT 2018}
}
Web of Science
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