Fabian, DM;
Ganose, AM;
Ziller, JW;
Scanlon, DO;
Beard, MC;
Ardo, S;
(2019)
Influence of One Specific Carbon–Carbon Bond on the Quality, Stability, and Photovoltaic Performance of Hybrid Organic–Inorganic Bismuth Iodide Materials.
ACS Applied Energy Materials
, 2
(3)
pp. 1579-1587.
10.1021/acsaem.8b01809.
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Abstract
Hybrid organic–inorganic halide perovskites are promising materials for thin-film solar cells. However, the toxicity and instability of best-in-class lead–halide perovskite materials make them nonideal. To combat these issues, we replaced lead with bismuth and explored the sensitivity of these new lead-free materials to the valency and bonding of their cationic organic groups. Specifically, we synthesized and characterized the materials properties and photophysical properties of hexane-1,6-diammonium bismuth pentaiodide ((HDA^{2+}Bil_{5}) and compared them to an analogue containing a more volatile organic group with half the number of carbon and nitrogen atoms in the form of n-propylammonium ((PA+)_{x}Bil_{3+x}, where 1<x<3). The full crystallographic structures of (HDA^{2+})Bil_{5} and (PA^{+})_{x}Bil_{3+x} were resolved by single-crystal X-ray diffraction. (HDA^{2+})Bil_{5} was shown to be pure-phase and have a one-dimensional structure, whereas (PA^{+})_{x}Bil_{3+x} was shown to be a mix of one-dimensional and zero-dimensional phases. Structures of the materials were confirmed by synchrotron X-ray diffraction of powders. Both (HDA^{2+})Bil_{5} and (PA^{+})_{x}Bil_{3+x} exhibit steady-state photoluminescence at room temperature. Density functional theory calculations of (HDA^{2+})Bil_{5} predict electronic absorption features and a ∼2 eV bandgap that are consistent with those observed experimentally. Structure–property relationships of the materials were examined, and moisture tolerance and film quality were found to be superior for dication-containing (HDA^{2+})Bil_{5} in relation to monocation-containing (PA^{+})_{x}Bil_{3+x}. We hypothesize that these trends are in part due to a molecular bridging effect enabled by the presence of the dicationic hexanediammonium groups in (HDA^{2+})Bil_{5}. Solar cells fabricated using (HDA^{2+})Bil_{5} as the photoactive layer exhibited photovoltaic action while those containing (PA^{+})_{x}Bil_{3+x} did not, suggesting that organic dicationic groups are beneficial to light-absorber morphology and ultimately solar-cell performance.
Type: | Article |
---|---|
Title: | Influence of One Specific Carbon–Carbon Bond on the Quality, Stability, and Photovoltaic Performance of Hybrid Organic–Inorganic Bismuth Iodide Materials |
Open access status: | An open access version is available from UCL Discovery |
DOI: | 10.1021/acsaem.8b01809 |
Publisher version: | http://doi.org/10.1021/acsaem.8b01809 |
Language: | English |
Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
Keywords: | bismuth halide, dications, hybrid organic−inorganic, nontoxic, photovoltaic, solar cells, solar fuels, stability |
UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
URI: | https://discovery.ucl.ac.uk/id/eprint/10073885 |
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